The development of mobile, noninvasive, and portable sensor technologies for diagnostics and emission control is highly demanded. For that purpose, laser carbonization is studied as a tool to produce responsive carbon materials from inexpensive organic precursors for the room-temperature selective detection of volatile organic compounds (VOCs) applicable in future sensor array-based devices. To increase the response of intrinsically low-responsive laser-patterned carbons (LP-C) to analytes in the gas phase, we tested carbonization in the presence of nanoscale ZnO precursors in primary inks. Following the addition of a zinc salt, Zn(NO3)2, a noticeable 43-fold increase in the sensor response (ΔR/R0 = −21.5% toward 2.5% acetone) was achieved. This effect is explained by a significant increase in the measurable surface area up to ∼700 m2·g–1 due to the carbothermic reduction supported by the in situ formation of ZnO nanoparticles. Varying Zn concentrations or the addition of as-prepared ZnO nanorods lead to different surface properties like the surface area, porosity, and polarity of LP-C. A predominant effect of the surface polarity on the selectivity toward different analytes of the sensors during physisorption, e.g., acetone vs toluene, was identified and tested. The best-performing LP-C sensors were finely characterized by transmission/scanning electron microscopies and X-ray photoelectron/energy-dispersive X-ray/Raman spectroscopies.