Metal–organic frameworks (MOFs) have been considered to be novel adsorbents for a variety of applications, because of their high surface areas, large pore volumes, tunable pore geometries, and versatile chemical compositions. Besides their applications in energy gas storage, such as H
2
and CH
4
, harmful gas removal has become an important potential area for MOFs applications. This chapter reviews recent research related to four different types of harmful gas adsorption in MOFs, including greenhouse gases such as CO
2
, inorganic toxic gases such as SO
x
, NO
x
, and NH
3
; volatile organic compounds such as benzene and formaldehyde; and radioactive gases such as Xe, Kr, and I
2
. This information is organized in a way that will attempt to introduce this attractive research area to a broad audience, as well as to reveal some trends and significant discoveries to the researchers who are interested in this area. Obviously, removing harmful gases can provide a cleaner and safer living environment to human beings and other creatures. MOFs as novel adsorbents possess advantages, such as high gas adsorption capacities and selectivities, as well as adjustable properties to suit specific needs. However, more fundamental work is still necessary to understand this topic better, and some challenges, such as cost and stability, are in the way of applying MOFs to practical applications.