Carbon micro/nanosphere-based surface molecularly imprinted adsorption material (SMIP@CS) has shown broad application prospects in the field of organic compound adsorption removal and recovery from liquid-phase environmental systems since it can meet all the separation requirements of high efficiency, deep level, identified selectivity, non-destructiveness, and recyclability. In this review, typical SMIP@CS materials applied in eco-environment field in past decade are reviewed. The general preparation methods and evaluation indices of SMIP@CS are summarized. Furthermore, by exploring the relationship between the matrix materials’ pore structures and adsorption properties of SMIP@CS towards organic compounds, the adsorption mechanism of SMIP@CS is deduced and confirmed. This work provides some theoretical support and practical experience for further research on imprinting matrix screening, imprinting method designing, and adsorption performance improving.