In this paper, a new junctionless graphene nanoribbon tunnel field-effect transistor (JLGNR TFET) is proposed as a multi-gas nanosensor. The nanosensor has been computationally assessed using a quantum simulation based on the self-consistent solutions of the mode space non-equilibrium Green’s function (NEGF) formalism coupled with the Poisson’s equation considering ballistic transport conditions. The proposed multi-gas nanosensor is endowed with two top gates ensuring both reservoirs’ doping and multi-gas sensing. The investigations have included the IDS-VGS transfer characteristics, the gas-induced electrostatic modulations, subthreshold swing, and sensitivity. The order of change in drain current has been considered as a sensitivity metric. The underlying physics of the proposed JLGNR TFET-based multi-gas nanosensor has also been studied through the analysis of the band diagrams behavior and the energy-position-resolved current spectrum. It has been found that the gas-induced work function modulation of the source (drain) gate affects the n-type (p-type) conduction branch by modulating the band-to-band tunneling (BTBT) while the p-type (n-type) conduction branch still unaffected forming a kind of high selectivity from operating regime point of view. The high sensitivity has been recorded in subthermionic subthreshold swing (SS < 60 mV/dec) regime considering small gas-induced gate work function modulation. In addition, advanced simulations have been performed for the detection of two different types of gases separately and simultaneously, where high-performance has been recorded in terms of sensitivity, selectivity, and electrical behavior. The proposed detection approach, which is viable, innovative, simple, and efficient, can be applied using other types of junctionless tunneling field-effect transistors with emerging channel nanomaterials such as the transition metal dichalcogenides materials. The proposed JLGNRTFET-based multi-gas nanosensor is not limited to two specific gases but can also detect other gases by employing appropriate gate materials in terms of selectivity.