Every episode of the show would find the Pussycats (along with Josie's boyfriend and band roadie Alan, their cowardly manager Alexander, Alexander's scheming sister Alexandra, and the equally scheming pet cat, Sebastian) en route to perform a gig or record a song in some exotic location. Somehow (often due to something Alexandra did) they would accidentally find themselves mixed up in an adventure/mystery. The antagonist was always a diabolical mad scientist, spy, or criminal who wanted to take over the world using some hi-tech device. The Pussycats would usually find themselves in possession of the plans for an invention, an item of interest to the villains, a secret spy message, etc., and the villains would give chase.

Towards the end of the episode, the villain would succeed in capturing the Pussycats and would begin executing their diabolical plan to take over the world. The gang would break free (usually thanks to Sebastian), and would proceed to "discombooberate" (their word) the device/lab and capture the bad guys. This would result in a final chase sequence, set to one of the songs recorded for the Capitol Records releases.

The Pussycats would succeed in capturing the villain and get back to their gig/recording session/etc. The final gag always centered around one of Alexandra's attempts to (a) interfere with/put an end to The Pussycats' performance, (b) steal Alan away from Josie, or (c) achieve both at the same time. More often than not, she would enlist Sebastian to carry out her dirty work, and Sebastian would always bumble the job in some way, which is unsurprising since he is a cat, and which would result in Alexandra getting in trouble and/or being made a fool of. Alexandra and Sebastian cat parallel another set of comic relief villains-Dick Dastardly and Muttley from Hanna-Barbera's Wacky Races. Sebastian even had the same laugh as Muttley, supplied by Don Messick.