Top Cat (or TC) is the yellow furred, greedy, somewhat lazy and clever main character. He wears a purple hat and vest. He often rips off and/or tricks his gang and Officer Dibble. He does respect the effort the gang does for him, but he often takes credit for it. That said, he is loyal to the gang and will help one of them if they need it. He also stops Officer Dibble from arresting him by lying to Dibble about how much talent Dibble has. He is voiced by Arnold Stang.
Top Cat's Gang
Benny is TC's right-hand man. He is short, innocent, chubby, naive and cute. A blue-coloured cat with a white sweater that fastens with a single button at his neck. His eyes are shown as black dots unlike the other cats who have white sclerae with black pupils. Benny may appear to be simple-minded, but he manages to ask the most logical questions during the gang's erratic endeavors. The gang relationship between Benny and TC is based on a devoted friendship between them. Benny the Ball is modeled after his voice actor Maurice Gosfield.
Choo-Choo, nicknamed Chooch to TC and the gang, is enthusiastic and devoted to TC even when he’s clueless as to what he’s doing. He is a pink cat with a white long-sleeve turtle-neck shirt, he is the tallest of the alley gang cats and often is depicted with the eyes of a Siamese cat. He lives at the fire house as the fire house cat as seen in one episode "Hawaii Here We Come". He had a couple of love crushes "Choo-Choo's Romance" and "Choo-Choo Goes Gaga-Gaga", however unlike Fancy-Fancy or Top Cat, Choo-Choo has no courage talking to girls. When he talks, his voice sounds like Woody Allen. He is voiced by Marvin Kaplan.
Brain appears to be a common henchman to Top Cat. Contrary to his name (which appears to have been given in jest or sarcasm), Brain is the dim-witted member of the alley gang, an orange cat with a violet T-Shirt with a black line. Brain is notorious for being unable to keep a secret and for his stuttering. He also seems to be in charge of the group's money (which they rarely have) and he runs up and down the road. Despite his apparent stupidity, he can sometimes say something brilliant, which TC instantly rephrases to make it sound like he said it. He is voiced by Leo De Lyon.
Fancy-Fancy also appears to be a common henchman to Top Cat. He is laid-back, sweet-talking and is regularly seen chatting up the ladies before leaving them when hearing the 'dustbin lid call'. A brown cat with a white scarf, he resembles Spook in appearance. His look and voice is based on Cary Grant. He is voiced by John Stephenson.
Spook is one of the most streetwise members of the gang. When he talks, a torrent of "like"'s are used. He is similar to Fancy-Fancy in demeanor and appearance, a sweet talking cat whose vernacular is based on that of a beatnik. When the gang need some help with a situation, he usually steps up to the plate. He is a pool shark with green fur and a torn black tie. He too is voiced by Leo De Lyon.
- Top Cat and his Alley Cats make cameos in the original Powerpuff Girls episode Catastroph. Which was around the time when Hanna-Barbera worked on the show.