We propose a crossed electric spin generation effect in multilayer structures. This effect combines the advantages of in-plane and gate electric fields for manipulating spin, and unveils a nice quantum geometric structure in terms of the underlying hybrid Berry curvatures that are unique to quasi-2D systems and manifest inherent spin-layer-orbital coupling. Combining our theory with first-principles calculations, we predict sizable spin generation in 2D ferromagnetic Fe3GeTe2 and altermagnetic V2Te2O. Our theory opens a new Berry-curvature route for all-electric spin manipulation in 2D materials