In the vibrant and fictional city of Tokyoko, known for its many nods to the creations of Tatsunoko Production, chaos reigns as the notorious Doronbo Gang wreaks havoc, seemingly demolishing a significant part of the landscape. However, the heroic duo known as Yatterman swiftly enters the scene, accompanied by their sentient dog-shaped mecha, Yatterwoof (voiced by Koichi Yamadera), and their whimsical robot sidekick, Toybotty. Through a series of entertaining and slapstick combat encounters, the Doronbo Trio eventually retreats to their mecha with the intent of defeating Yatterman. In a moment of accidental celebration, the villains trigger their mecha's self-destruct mechanism, leading to a chaotic aftermath where a teenage girl emerges from the rubble clutching a mysterious blue object.
The narrative unfolds as the Narrator (voiced by Koichi Yamadera) shares the backstory of Gan Takada (a.k.a. Yatterman #1, played by Sho Sakurai) and his girlfriend, Ai Kaminari (a.k.a. Yatterman #2, portrayed by Kyoko Fukada). They lead a double life as defenders of justice while being rooted in the establishment of Takada Toys, a company founded by Gan's father. Demonstrating exceptional ingenuity, Gan created Toybotty and revived the legacy of Yatterwoof as an abandoned project from his father. The girl, named Shoko Kaieda (portrayed by Anri Okamoto), is revealed to be the daughter of Dr. Kaieda (played by Sadawo Abe), an archaeologist on a quest to locate the fragments of a legendary artifact known as the Skull Stone. This mystic object has been split into four segments, and danger lurks as Dr. Kaieda is assaulted in the ominous Narway Forest by a menacing entity named Skullobey.
The introduction of the Doronbo Gang adds a delightful charm to the unfolding chaos. This motley crew includes the alluring and cunning boss, Doronjo, the clever yet lecherous mecha genius Boyacky (played by Katsuhisa Namase), and the stout strongman Tonzuraa (portrayed by Kendô Kobayashi). At the behest of Skullobey, they embark on a mission to reclaim the Skull Stone fragments, aware of the severe repercussions that await them should they falter. To finance their ambitious plans for a new mecha known as the Bridesmaidiot (Virgin Roader), they creatively set up a wedding shop named Doro Merry. Their leader, Doronjo, is fervently committed to fulfilling Skullobey's wishes, receiving messages about the whereabouts of the remaining stone pieces, with one reported to be in Ogypt.
As the quest intensifies, the trio unwittingly comes under the watchful eye of Toybotty, who keeps Gan and Ai updated on their mischievous escapades. Upon discovering the slice of the Skull Stone, the Yatterman duo springs into action, setting off for Ogypt. However, the Doronbo Trio's repeated attempts to dispatch them using their mecha yield humorous yet disastrous results, leading to Yatterwoof being ensnared in a failed heist involving a bottle of Mechanade.
Back at their hideout, the conflict deepens as Gan strives to repair Yatterwoof, while Ai, filled with jealousy towards Shoko and the alluring Doronjo, sets out for a reflective stroll. Misfortune strikes when the trio receives news of another piece located in the enigmatic Southern Halps, as it comes to light that Skullobey harbors romantic intentions for Doronjo. Meanwhile, a shadow of worry looms as items across the globe start to mysteriously vanish, and in the midst of uncovering the truth about the Skull Stones, Toybotty vanishes as well.
In a twist of fate, Ai uncovers another of the villains' schemes involving a sushi restaurant, which is a ploy to fund their colossal squid mecha. After eavesdropping on their plans, she learns the location of the last fragment hidden in the Southern Halps. With that knowledge, the Doronbo Trio gears up in their new Squid Mecha.
Returning to their base means delving deeper into the chaotic mayhem. Gan reads Toybotty's final analyses before its disappearance: if the Skull pieces are united, they will unleash a force capable of obliterating time itself, leading to universal nullification. The Yatterman duo bravely embarks on another mission with Shoko accompanying them on an upgraded Yatterwoof, now called Yatterking. Conflict arises once more when the villains arrive just as they find the missing piece, and the Yatterman duo becomes ensnared in a mechanical prison arranged by Skullobey.
In a climactic showdown, Doronjo zaps Ai to divide the heroes, only to witness the undeniable bond that exists between Gan and Ai. With Shoko's plea, Dr. Kaieda manages to break free from Skullobey's control, revealing his true form. In an extraordinary display of teamwork, Yatterman #1 and #2 join forces with their reformed adversaries, the Doronbo Gang, to vanquish Skullobey, securing him into another realm.
Eventually, the story concludes with Gan and Ai bidding farewell to Shoko and her father, who set off on their global adventures, while the Doronbo Gang parts ways. Yet, the threads of their destinies intertwine, suggesting a hopeful reunion on the horizon, implying that their journeys are tied together on this winding road of camaraderie and mischief.