Zeolites are the most important technological materials made up of framework of aluminosilicates, aluminophosphates, vanadophosphates, silicoaluminophosphates and so on. In the recent years the interest is being extended greatly from the molecular sieves to selective catalysis, gas adsorption, nanoparticle hosts, atmospheric ecosystems, etc. These aluminophosphate molecular sieve zeolites have uni-, two-, and three-dimensional channels which are obtained hydrothermally in the presence of organic amines as structure directing agents. VPI-5 is an important aluminophosphate molecular sieve with 18 tetrahedral rings and free diameter of 12.1 A. In this paper, the authors discuss the synthesis of R+3: aluminophosphate, where R=Ce, Pr and Nd.