AbstractIn this research, the ultrasound (US) technique was applied as a facile synthesis method for preparing the black TiO2‐g‐C3N4 type II heterojunction, coupled with a Schottky junction MOF (ZIF‐67)‐derived x wt% Co3S4/nitrogen‐doped carbon (NC) (x = 3, 10, and 15) with hollow nanobox (HNB) morphology, as a smart nanoheteroarchitecture (NHA) photocatalyst to enhance visible‐light photocatalytic activity. Additionally, the solvothermal synthesis route was employed to fabricate the MOF (ZIF‐67)‐derived Co3S4/NC cubic hollow nanoboxes (CHNBs) before the pyrolysis process. The black TiO2‐g‐C3N4 wt% Co3S4/NC (TiCN‐15% CoS/NC) NHAs exhibited high photocatalytic activity in degrading methylene blue. The synergetic effect of all components in black TiCN‐x wt% CoS/NC NHAs resulted in efficient electron‐hole pair separation and charge mobility on Co3S4/NC HNB and g‐C3N4 surfaces, which led to a highly effective recombination rate of charge carriers and an excellent improvement in photocatalytic performance.