Chemiresistive gas sensors are extensively employed in environmental monitoring, disease diagnostics, and industrial safety due to their high sensitivity, low cost, and miniaturization. However, the high cross-sensitivity and poor selectivity of gas sensors limit their practical applications in complex environmental detection. In particular, the mechanisms underlying the selective response of certain chemiresistive materials to specific gases are not yet fully understood. In this review, we systematically discuss material design strategies and system integration techniques for enhancing the selectivity and sensitivity of gas sensors. The focus of material design primarily on the modification and optimization of advanced functional materials, including semiconductor metal oxides (SMOs), metallic/alloy systems, conjugated polymers (CPs), and two-dimensional nanomaterials. This study offers a comprehensive investigation into the underlying mechanisms for enhancing the gas sensing performance through oxygen vacancy modulation, single-atom catalysis, and heterojunction engineering. Furthermore, we explore the potential of emerging technologies, such as bionics and artificial intelligence, to synergistically integrate with functional sensitive materials, thereby achieving a significant enhancement in the selectivity of gas sensors. This review concludes by offering recommendations aimed at improving the selectivity of gas sensors, along with suggesting potential avenues for future research and development.