In a method of synthesizing a silicoaluminophosphate molecular sieve having 90%+CHA framework type character, a reaction mixture is prepared comprising first combining a reactive source of aluminum with a reactive source of phosphorus to form a primary mixture that is aged. A reactive source of silicon and a template for directing the formation of the molecular sieve can then be added to form a synthesis mixture. Crystallization is then induced in the synthesis mixture. Advantageously, (i) the source of silicon comprises an organosilicate, (ii) the source of phosphorus optionally comprises an organophosphate, and (iii) the crystallized silicoaluminophosphate molecular sieve has a crystal size distribution such that its average crystal size is not greater than 5 μm. The molecular sieve can then preferably be used in a hydrocarbon (oxygenates-to-olefins) conversion process.