Graphene materials synthesized using direct laser writing (laser-induced graphene; LIG) are fa-vorable sensor materials because of their large surface area, ease of fabrication, and cost effec-tiveness. In particular, LIG decorated with metal nanoparticles (NPs) has been used in various sensors, including chemical sensors and electronic and electrochemical biosensors. However, the effect of metal decoration on LIG sensors remains controversial; hypotheses based on computa-tional simulations do not always match experimental results, and even experimental results re-ported by different researchers have not been consistent. In the present study, we explored the effects of metal decorations on LIG gas sensors, with NO2 and NH3 gases as representative oxi-dizing and reducing agents, respectively. To eliminate unwanted side effects arising from metal salt residues, metal NPs were directly deposited by vacuum evaporation. Although the gas sen-sitivities of the sensors deteriorate upon metal decoration irrespective of the metal work function in the case of NO2 gas, they improve upon metal decoration in the case of NH3 exposure. A careful investigation of the chemical structure and morphology of the metal NPs in the LIG sensors shows that the spontaneous oxidation of metal NPs with a low work function changes the be-havior of the LIG gas sensors and that the sensor behaviors under NO2 and NH3 gases follow different principles.