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Cesium lead halide (CsPbX3) perovskite quantum dots (PQDs) instability is solved by sealing them in 3D form double-layered mesoporous silica nanospheres (3D-MSNs) with uniform particle size. When compared to other commercial 2D mesoporous silica materials, 3D-MSNs can better encapsulate PQD precursors within their pores. After introducing CsX and PbX2 into 3D-MSN pores, calcination provides simultaneous production of CsPbX3 and coverage for outer-layer 3D-MSN pores, resulting in the formation of a water and light-resistant CsPbX3@3D-MSNs composite material. The growth mechanism of PQDs inside 3D-MSNs and their thermal phase structure behavior are deeply studied. Heating and cooling at 25–350 °C affects the crystal phase of PQDs (δ, α, β, and γ) and their photoluminescence properties. The CsPbX3@MSNs composite material exhibits high stability and dispersity, making it suitable for light-emitting diodes and stretchable, self-healable, luminescent thin films.