Composites of a crystalline or long-ranged ordered material (CLROM), for example zeolites and non-zeolitic molecular sieves, are disclosed. The composites have both a macroscopic particle size (e.g., an average particle size of greater than about 0.1 mm), as desired in commercial applications, as well as improved functionality. Such composites result from the conversion of a conventional amorphous material, for example a solid amorphous silica alumina of this particle size, into the CLROM. According to particular embodiments, all or substantially all (e.g., at least about 99%) of the amorphous material is converted to the CLROM, such that essentially the entire macroscopic material may have the desired functionality of the CLROM as a catalyst or adsorbent.