Designing a semiconductor‐based heterostructure photocatalyst for achieving the efficient separation of photogenerated electron‐hole pairs is highly important for enhancing H2 releasing photocatalysis. Here, a new class of Ni1−xCoxSe2–C/ZnIn2S4 hierarchical nanocages with abundant and compact ZnIn2S4 nanosheets/Ni1−xCoxSe2C nanosheets 2D/2D hetero–interfaces, is designed and synthesized. The constructed heterostructure photocatalyst exposes rich hetero‐junctions, supplying the broad and short transfer paths for charge carriers. The close contacts of these two kinds of nanosheets induce a strong interaction between ZnIn2S4 and Ni1−xCoxSe2C, improving the separation and transfer of photo‐generated electron‐hole pairs. As a consequence, the distinctive Ni1−xCoxSe2C/ZnIn2S4 hierarchical nanocages without using additional noble‐metal cocatalysts, display remarkable H2‐relaesing photocatalytic activity with a rate of 5.10 mmol g−1 h−1 under visible light irradiation, which is 6.2 and 30 times higher than those of fresh ZnIn2S4 nanosheets and bare Ni1−xCoxSe2C nanocages, respectively. Spectroscopic characterizations and theory calculations reveal that the strong interaction between ZnIn2S4 and Ni1−xCoxSe2C 2D/2D hetero‐interfaces can powerfully promote the separation of photo‐generated charge carriers and the electrons transfer from ZnIn2S4 to Ni1−xCoxSe2C.