The present review article summarizes the recent findings reported in the literature with regard to the use of molecularly imprinted polymers for the removal of arsenic from water and wastewater. MIPs are polymers in which a template is employed in order to enable the formation of recognition sites during the covalent assembly of the bulk phase, via a polymerization or polycondensation process. The efficiency of both arsenic species and the mechanism of removal are highlighted. The results have shown that under certain conditions, MIPs demonstrated arsenic sorption capacities of up to 130 mg/g for As(V) and 151 mg/g for As(III), while the regeneration ability was found to reach up to more than 20 cycles. The overall results showed that further development of MIPs could result in the formation of promising adsorbents for arsenic removal from waters. The use of MIPs for the removal not only of arsenic but also other inorganic contaminants is considered a very important topic, with great potential in terms of future applications in water treatment. The main advantage of these materials is that they are very selective toward the contaminant of interest. This enhanced selectivity is attributed to the incorporation of specific templates, which can then adsorb the contaminant of interest almost exclusively. Therefore, the main problem in adsorption processes is the competition for adsorption sites by other water components, for example, phosphates, nitrates, carbonates, and sulfates, which can be circumvented by the use of MI-type adsorbents.