Reported here are two highly porous examples of MOCOFs, a new family of framework materials seamlessly integrating the coordinate bonds of metal-organic frameworks (MOFs) and covalent bonds of covalent organic framework materials (COFs). These two materials represent the lightest zeolite RHOs. Their synthesis is an extraordinary example in which the structure-directing effect of the substituent groups on the cross-linking imidazolyl ring strikes a perfect balance with their pore narrowing effect, leading to the creation of a very open zeolite RHO topology with highly accessible internal pores, characterized by a large surface area of 1818 m(2)/g and a high CO2 storage capability as high as 35.6 cm(3)/g at 760 Torr and 273 K.