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Active tether and transportation of cargoes on cytoskeletal highway enabled by molecular motors is key for accurate delivery of vesicles and organelles in the complex intracellular environment. Here, a hybrid system composed of colloidal motors and self‐assembled lipid tubes is designed to mimic the subcellular traffic system in living cells. The colloidal motors, composed of gold‐coated hematite, display light‐activated self‐propulsion tunable by the light intensity and the concentration of hydrogen peroxide fuel. Importantly, the motors show light‐switchable binding with lipid cargoes and attachment to the lipid tubes, whereby the latter act as the motor highways. Upon assembly, the colloidal motor/lipid tube system demonstrates directional delivery of lipid vesicles, emulating intracellular transportation. The assembly and function of the hybrid system are rationalized by a cooperative action of light‐triggered electrophoretic and hydrodynamic effects, supported by finite element analysis. A synthetic analog of the biological protein motor/cytoskeletal filament system is realized for the manipulation and delivery of different matter at the microscale, which is expected to be a promising platform for various applications in materials science, nanotechnology, microfluidics, and synthetic biology.

Light‐actuated micromachines are of enormous interest due to their ability to harvest light for triggering catalytic reactions to acquire free energy for mechanical work. This work presents an inorganic–organic hybrid copolymeric poly(cyclotriphosphazene‐co‐barbituric acid) colloid, which displays multiwavelength excited emission and catalytic activities, exploiting the unique structural, chemical, and optical features of inorganic heterocyclic ring hexachlorocyclotriphosphazene and organic co‐monomer barbituric acid. Specifically, this work reveals particle‐resolved unusual multicolor emission under excitation with the same or different wavelengths of light using fluorescence microscopy. The result is rationalized by density functional theory studies. In this work, the authors find that emission is coincident with fluorometric measurements, and the photocatalytic properties are anticipated from the overall band structure. This work also demonstrates the use of these colloids as micropumps, which can be remotely activated by UV, blue, and green lights under fuel‐free conditions, and ascribe the behavior to ionic diffusiophoresis arising from light‐triggered generation of H+ and other charged species. This work offers a new class of polymeric colloids with multiple‐wavelength excited emission and catalytic activities, which is expected to open new opportunities in the design of fuel‐free, photo‐actuated micromachines and active systems.