The demand for highly functional chemical gas sensors has surged due to the increasing awareness of human health to monitor metabolic disorders or noncommunicable diseases, safety measures against harmful greenhouse and/or explosive gases, and determination of food freshness. Over the years of dedicated research, several types of chemiresistive gas sensors have been realized with appreciable sensitivities toward various gases. However, critical issues such as poor selectivity and sluggish response/recovery speeds continue to impede their widespread commercialization. Specifically, the mechanisms behind the selective response of some chemiresistive materials toward specific gas analytes remain unclear. In this review, we discuss state-of-the-art strategies employed to attain gas-selective chemiresistive materials, with particular emphasis on materials design, surface modification or functionalization with catalysts, defect engineering, material structure control, and integration with physical/chemical gas filtration media. The nature of material surface-gas interactions and the supporting mechanisms are elucidated, opening opportunities for optimizing the materials design, fine-tuning the gas sensing performance, and guiding the selection of the most appropriate materials for the accurate detection of specific gases. This review concludes with recommendations for future research directions and potential opportunities for further selectivity improvements.