The invention discloses a method of solid-phase synthesis of an AEI-structure molecular sieve. The method includes the following steps: 1) performing a mixed reaction to an aluminum source with an alkyl piperidinium organic template agent and performing pressure reduced distillation to remove residual water to prepare an ammonium metaaluminate compound gel; 2) performing a crystallization reaction to the gel with a mixture, which is produced by mixing and grinding a silicon source, an alkaline source and a molecular sieve seed crystal to produce raw powder of the AEI-structure molecular sieve. The method is high in synthesis yield, is short in crystallization time, is reduced in usage amount of the solvent and template agent, and is suitable for large-scale industrial production. When the raw powder of the AEI molecular sieve is exchanged with metal cations, a metal-AEI molecular sieve is produced, which can be applied to a catalytic reduction reaction of NOx in tail gas; and when the raw powder of the AEI molecular sieve is exchanged with and activated by ammonium ion, a hydrogen-type AEI molecular sieve is produced, which can be used in a MTO reaction to produce low-carbon olefins at high yield.