Janus Zn/Au micromotors (MMs) are fabricated by sputtering Au onto one hemisphere of Zn microparticles, resulting in spherical light-responsive structures with dual photothermal propulsion and SERS detection capabilities. Zn/Au MMs exhibit efficient propulsion under near-infrared (NIR) light, with motion driven through thermophoretic effects induced by local heating of the Au surface. The MMs are activated by CARS microscopy, enabling label-free, real-time trajectory tracking, with propulsion velocities increasing linearly with total laser power and remaining largely independent of the pump wavelength within the NIR range (780–900 nm) under dual-wavelength excitation. A 30 nm Au coating provides the optimal balance between optical absorption and propulsion efficiency, while independent modulation of the pump and Stokes beams confirms that dual-beam excitation is essential for sustained motion. Zn/Au MMs work perfectly as active SERS platforms for single and multiplex detection of the anticancer drugs methotrexate (MTX) and 6-mercaptopurine (6-MP). Their active motion enhances analyte exchange at the Au surface, reducing affinity-driven saturation and competitive adsorption effects, which broadens the linear range and improves multiplex SERS detection. The integration of autonomous motion with chemometrics models, including partial least squares-discrimination analysis (PLS-DA) on the obtained SERS data, represents a promising step toward MM-based diagnostic systems.