The organic fraction of municipal solid waste (OFMSW) is a widely-available promising feedstock for biofuel production. However, the presence of different inhibitors originating from fruit and food/beverage wastes as well as recalcitrant lignocellulosic fractions hampers its bioconversion. This necessitates a pretreatment to augment the biodigestibility and fermentability of OFMSW. Hence, this review aims to provide the in-vogue inhibitory compound removal and pretreatment techniques that have been employed for efficient OFMSW conversion into biofuels, i.e., hydrogen, biogas, ethanol, and butanol. The techniques are compared concerning their mode of action, chemical and energy consumption, inhibitor formation and removal, economic feasibility, and environmental sustainability. This critique also reviews the existing knowledge gap and future perspectives for efficient OFMSW valorization. The insights provided pave the way toward developing energy-resilient cities while addressing environmental crises related to generating OFMSW.