Like previous games in the series, players primarily control Sly Cooper, who must sneak around and navigate various obstacles to help restore the history of the Thievius Raccoonus. Many of Sly's abilities return, such as navigating poles and ropes, jumping across narrow platforms and stealing items from guards. New to this game are costumes earned throughout the course of the game, which give Sly access to new abilities. Examples include a suit of armor that allows Sly to reflect projectiles with a shield, an archery outfit that lets him shoot arrows at targets to create rope lines, and an Arabian pirate-like suit that allows him to slow down time and use a sword to break sturdy objects. These costumes can be taken to previously visited levels to reach secret areasNew secret masks and treasures are hidden throughout the game; the latter item, unlike its counterpart in previous installments, is collectible only and cannot be sold on the game's ThiefNet service (although the player still receives an in-game monetary reward). The clue bottles from Sly Cooper and the Thievius Raccoonus and Sly 2: Band of Thieves make a return, allowing the player to unlock new abilities for all of the playable characters. A new feature allows anyone who owns both the PlayStation Vita and PlayStation 3 versions of the game to use the Vita system as "a set of x-ray goggles" to find any of these hidden collectibles anywhere in the world, through the use of augmented reality. The binary characters displayed during Bentley's plans are ASCII-encoded text messages and can be decoded manually.
Bentley, Murray, and Carmelita Fox return as playable characters, along with some of Sly's ancestors, who each possess unique abilities. Worlds in the game are claimed to be three times the size of the original trilogy. The game also supports stereoscopic 3D and local multiplayer in some sections of the game.