The Wild Wild Pussycats accept Makoto Tsukauchi's invitation to participate in the Captain Celebrity's farewell show at the Tokyo Sky Egg, where they perform a choreography. The Tokyo Sky Egg is attacked by Bombers, sent there by villain Number 6 to assassinate Captain Celebrity.
Students from U.A. High travel to the Pussycats' reserve to train over the summer. Tiger and the Wild, Wild Pussycats introduce themselves to Class 1-B on the second day of camp. While the girls introduce themselves by explaining their Quirks, Tiger says that he has the ability to defeat and dismantle anyone in a fight.
Tiger instructs all power-up and strength-oriented students to train with him and already has Izuku Midoriya stretching repeatedly. He confronts Izuku and asks him to attack, easily avoiding and countering Izuku's attempt to land a 5% Detroit Smash and sending him flying into a tree, noting that his muscles are not ripping apart yet, thus not getting stronger. He continues training and encouraging Izuku, while Kota Izumi silently watches them from behind a tree.
The next day, Tiger catches Izuku talking his teacher Shota Aizawa. He confronts Izuku and says he is not going beyond. That night, he and the others notice the mountain has been set on fire, and are caught off guard when Pixie-Bob is attacked by Magne and Spinner. Izuku tries to rush to her side, but Tiger cuts him off and faces off against the villains.
Once Kenji threatens to kill Pixie-Bob, he says that he will not let him. After Shuichi interrupts them and introduces himself, Yawara angrily reprimands him for scarring Ryuko's face.
Both Tiger and Mandalay fight Kenji and Shuichi respectively. When Kenji sees Shuichi having trouble dealing with Shino and uses her Quirk to pull Shino towards her, Yawara lands a surprise punch on her, freeing Shino from her grasp. He then punches her again, but this time Kenji manages to block his attack. While getting up, Shino informs Yawara that she cannot communicate with Ragdoll, which she considers strange since she normally answers her immediately. Yawara continues fighting Kenji and holds his own, managing to immobilize her by wrapping his arms around the villain. Yawara and Shino plan to take in Kenji and Shuichi, but Kurogiri appears and rescues the two villains.
Two days later, Yawara joins the Police Force and a large number of Pro Heroes in the rescue operation of Katsuki Bakugo. Yawara states that his teammate Tomoko was kidnapped by the Vanguard Action Squad and that he will rescue her; he notes the League of Villains has a number of hideouts instead of one.
Yawara, Mt. Lady, Best Jeanist, and Gang Orca infiltrate the partially destroyed warehouse and apprehend all the Nomus while Yawara rescues Tomoko. Hakamada informs Naomasa Tsukauchi that the warehouse has been cleared.
Yawara attempts to speak to Tomoko but she is unresponsive. Suddenly, All For One appears in the shadows and apologizes to Yawara, explaining that he stole Ragdoll's Quirk. Before the Pro Heroes can act, All For One destroys the warehouse while damaging the surrounding area. Hakamada reacts quickly and manipulates his fellow Pro Heroes' clothes, causing Yawara to be reeled back, allowing him to survive All For One's attack. However, Yawara is still heavily injured by the attack. While Edgeshot and Endeavor assist All Might, Yawara rescues the trapped civilian whom All Might was protecting in order to alleviate his burden.
After All Might defeats All For One, Yawara returns home. The Pussycats comfort a crying Tomoko after her hero license was suspended due to losing her Quirk.
When the Pussycats visited U.A., Yawara and his team introduced themselves to the students again before giving them chocolate his friends made. He apologizes to Katsuki for not properly protecting him when he was kidnapped, but the latter tells him not to worry himself.
As he gives out tea, Rikido asks why the Pussycats have decided to pay them a visit. They reply that they came to celebrate Ragdoll's reinstatement to provide support for the Pussycats, at least as a secretary, due the loss of her Quirk. They are informed that All For One cannot transfer the Quirk he stole back to its original user or to another person
Momo wonders why the Pussycats would rejoin at this time. They state that the Hero Billboard Chart JP will be broadcasted and that they are 411th on the billboard chart. Eijiro assumes that the Pussycats have returned so that they can rank higher, to which they refute and reply that despite everything, they’re coming off their hiatus because there are still many fans who support them and want to see them back in action. 
Next year, by the end of March, thanks to the police investigations, and the information leaked by Hawks, who was acting as a spy, the Hero Public Safety Commission organize the Heroes and the Police Force to take down the Paranormal Liberation Front. The Pussycats participates with other heroes in a meeting where Detective Naomasa informs them about Dr. Kyudai Garaki, the current board chairman of Jaku General Hospital, is an ally of Tomura Shigaraki and the creator of the Nomu, and that there is a section of the hospital that only he can access. 
The Pussycats are part of the team of heroes led by Endeavor in charge of raiding on Jaku General Hospital. While one group, of which the Pussycats are part, are in charge of evacuating patients, visitors and hospital staff from the building, another group is in charge of arresting Garaki, although the situation gets complicated when he releases a horde of Nomu to escape to his secret laboratory and awaken Tomura from his stasis.
Regardless, the heroes manage to defeat all the creatures, storm the laboratory, and arrest Garaki before he could awaken Tomura. It seemed that the mission had successfully ended, but at that moment Tomura awakens and uses his Decay. The Decay spreads through the hospital, completely disintegrating it and killing several heroes who were trying to flee. However the destruction does not stop but continues to spread.