The electronic transport properties of the four carbon isomers: graphene+, T-graphene, net-graphene, and biphenylene, as well as the gas-sensing properties to the nitrogen-based gas molecules including NO 2 , NO, and NH 3 molecules, are systematically studied and comparatively analyzed by combining the density functional theory with the nonequilibrium Green's function. The four carbon isomers are metallic, especially with graphene+ being a Dirac metal due to the two Dirac cones present at the Fermi energy level. The two-dimensional devices based on these four carbon isomers exhibit good conduction properties in the order of biphenylene > T-graphene > graphene+ > netgraphene. More interestingly, net-graphene-based and biphenylene-based devices demonstrate significant anisotropic transport properties. The gas sensors based on the above four structures all have good selectivity and sensitivity to the NO 2 molecule, among which T-graphene-based gas sensors are the most prominent with a maximum ΔI value of 39.98 μA, being only three-fifths of the original. In addition, graphene+-based and biphenylene-based gas sensors are also sensitive to the NO molecule with maximum ΔI values of 29.42 and 25.63 μA, respectively. However, the four gas sensors are all physically adsorbed for the NH 3 molecule. By the adsorption energy, charge transfer, electron localization functions, and molecular projection of self-consistent Hamiltonian states, the mechanisms behind all properties can be clearly explained. This work shows the potential of graphene+, T-graphene, net-graphene, and biphenylene for the detection of toxic molecules of NO and NO 2 .