A mesoporous composite (FZ) comprising microsheets of hematite modified and decorated with tetragonal zirconia nanocrystallites (∼4nm size), useful for adsorbing cationic pollutants from water, is prepared by a hydrothermal method. It exhibits improved adsorption behavior for methylene blue (MB) and various heavy metal ions (>99% efficiency for Cu2+, Cd2+ and Pb2+, initial concentration C0=5–20mg/L) as compared to unmodified zirconia (Z0) and hematite (F0). This behavior of FZ is ascribed to a combination of surface features: its high zeta potential ζ=−50.7mV (∼1.8 times more negative than ζ of Z0 or F0) and large number of mesopores (size distribution 1.8–33nm, maxima at 3.1nm) leading to a reasonably high surface area (100.5m2/g). For MB adsorption (C0=5–40mg/L), correlation coefficient (R2) values for different adsorption isotherm models are in the order Langmuir (0.990)> Temkin (0.956)> Freundlich (0.842), indicating homogeneous FZ surface which supports a monolayer of MB. Maximum monolayer adsorption capacity Qm, Freundlich constant KF (related to adsorption capacity) and Temkin constant bT (related to adsorption heat) are 44.7mg/g, 12.8 (mg/g)(L/mg)1/f and 257.8J/mol, respectively (1/f=heterogeneity factor). Pb2+ adsorption conforms well to both the Langmuir and Freundlich models (R2>0.99), with Qm=34.3mg/g. Much higher KF=75.0 (mg/g)(L/mg)1/f and bT=665.2J/mol (R2=0.941 for Temkin model) in this case indicates a significantly favorable Pb2+ adsorption. FZ exhibits reasonably good reusability for 3–4 cycles of use for MB/Pb2+ adsorption.