A sensitive photodetector of graphene nanocrystallites embedded carbon (GNEC) film coated on p‐silicon has been proposed. Different from the conventional growth mode of graphene, GNEC film contains a large amount of vertically grown graphene nanocrystallites (GNs). Edges of GNs act as electron trapping centers, increasing the ability to capture electrons. Different types of films are prepared under various deposition biases (20, 40, 60, and 80 V), which have different density of edges (Nedge). Edge entrapment improves the photocurrent responsivity of 40 V film (high Nedge) to 0.401 A W−1, compared with 0.126 A W−1 of 20 V film (amorphous, no Nedge) and 0.194 A W−1 of 80 V film (low Nedge). A high specific detectivity of 1.34 × 1012 cm Hz1/2 W−1 is exhibited at zero bias. GNs maintain a charge transport channel, which makes it have a fast response time τrise = 260 ns.