Effective control of toxic gaseous pollutants being emitted into the atmosphere has posed a critical and urgent challenge to deal with global climate change, protect the environment and human health as well as achieve clean and sustainable development. There remains a continuous threat to our human life from various toxic gaseous chemicals. Traditional methods for removing toxic gases usually suffer from shortcomings, such as low-capacity, energy-intensive, waste generation, and high cost. Metal-organic frameworks (MOFs), architected by various metal centers and organic ligands, represent a new type of adsorbent, which could readily offer a promising solution to capturing toxic gases. In this review, we provide detailed insights of the recent progress made on the adsorptive capture performance of MOF materials towards several critical toxic gases, such as SO₂, NO₂, NH₃, H₂S, sarin, CNCl, and CO. Considering the working condition and mixture components, the adsorption performance of various toxic gases are critically assessed and sorted. By comparing different modification strategies of a series of MOFs and corresponding performance manifestations, we make attempts to delineate future research directions to improve the adsorptive capture performance of MOFs toward toxic gases for real industrial applications.