Manganese-intercalated layered tantalotungstates have been assembled by tantalotungstatete nanosheets with manganese ions via an exfoliation-restacking route.The as-prepared nanohybrids are mesoporous with specific surface areas more than 36 m2/g and the mesopores are originated from the house-of-cards-type stacking of the intercalated crystallites.Introducing manganese ions into the intersheeted regions allows the nanohybrids to exhibit distinct spectral responses in visible-light region with band gaps less than 2.54 eV.The porous nanohybrids exhibit high photocatalytic activities in the degradation of methylene blue under visible-light irradiation.