Twilight Syndicate is an adventure game where players take on the role of a rookie Interpol detective tracking criminals across the globe. Armed with only a initial clue, players must investigate locations, follow trails, and piece together evidence to capture their targets. Along the way, they uncover the secrets of the Twilight Syndicate, a shadowy organization tied to legendary heists.

Twilight Syndicate offers a campaign mode where players solve cases and uncover the truth about the Twilight Syndicate. The game begins with the player receiving a clue that leads them to a specific location. Players travel, talk to NPCs, and investigate for more leads. Each location presents challenges like finding hidden clues or solving puzzles.

The game focuses on exploration, deduction, and decision-making. Every choice matters, keeping players engaged as they uncover the Twilight Syndicate's secrets and get closer to capturing the main antagonist initially know as "The Gentleman".