With the unique advantages of lower operational and maintenance cost, the applications of subsurface flow constructed wetlands for the treatment of wastewater have been increasing rapidly throughout the world. The removal of nitrogen and organics by such systems has gained substantial attention in recent years. In subsurface flow wetlands, the removal of pollutants often relies on a diverse range of co-existing physical, chemical and biological routes, which are vitally dependent on numerous environmental and operational parameters. This paper provides a comprehensive review of wetland structures, classic and novel nitrogen and organics removal mechanisms along with the key environmental parameters and operational conditions that enhance removal in subsurface flow wetland systems. The critical exploration identifies the major environmental parameters such as: pH, DO, and temperature, operational factors i.e. organic carbon availability, loading, feed mode, retention time, recirculation, harvesting, and the complex role (of both parameters) on classical nitrogen and organics removal pathways. Subsequently, the necessity of further extensive research on such factors, for promoting novel nitrogen removal routes in wetland systems has also been highlighted. The expansion of the review on the influence of the unconventional wetland matrix indicates that, the structural differences and inherent properties of these media can support substantial nitrogen and organics removal from wastewater, under optimal operating conditions. Overall, the critical review illustrates the necessity of a profound knowledge on the complicated inter-relationship between nitrogen and organics removal routes, governing environmental and operational parameters, and wetland matrix for improving the treatment performances of subsurface flow wetlands.