The integration of organic and inorganic building blocks into novel nanohybrids is an important tool to exploit innovative materials with desirable functionalities. For this purpose, carbon nanotube--nanoparticle nanoarchitectures are intensively studied. We report here an efficient noncovalent chemical route to density-controllably and uniformly assemble single-walled carbon nanotubes with CdS nanoparticles. The methodology not only promises the resulting hybrids will be solution-processable but also endows the hybrids with distinct optoelectronic properties including tunable photoresponse mediated by amine molecules. On the basis of these merits, reliable thin-film photoswitches and light-driven chemical sensors are demonstrated, which highlights the potential of tailored hybrids in the development of new tunable optoelectronic devices and sensors.