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Pharmaceutical contamination threatens both humans and the environment, and several technologies have been adapted for the removal of pharmaceuticals. The coagulation-flocculation process demonstrates a feasible solution for pharmaceutical removal. However, the chemical coagulation process has its drawbacks, such as excessive and toxic sludge production and high production cost. To overcome these shortcomings, the feasibility of natural-based coagulants, due to their biodegradability, safety, and availability, has been investigated by several researchers. This review presented the recent advances of using natural coagulants for pharmaceutical compound removal from aqueous solutions. The main mechanisms of natural coagulants for pharmaceutical removal from water and wastewater are charge neutralization and polymer bridges. Natural coagulants extracted from plants are more commonly investigated than those extracted from animals due to their affordability. Natural coagulants are competitive in terms of their performance and environmental sustainability. Developing a reliable extraction method is required, and therefore further investigation is essential to obtain a complete insight regarding the performance and the effect of environmental factors during pharmaceutical removal by natural coagulants. Finally, the indirect application of natural coagulants is an essential step for implementing green water and wastewater treatment technologies.