Compositing has been the main approach for material creation via wisely combining material components with different properties. MnO2 nanosheets (MNSs) with thin 2 D morphology are usually applied to composite molecules or nanomaterials for biosensing and bioimaging applications. However, such composition is actually structurally unmatched, albeit performance matching. Here, a series of benefits merely on the basis of structural match have been unearthed via tailoring MNSs with four sizes by synthesis under controllable hypergravity field. The classical fluorophore-quencher couple was utilized as the subject model, where the soft supramolecular nanogels based on aggregation-induced emission (AIE)-active gold nanoclusters were wrapped by MNSs of strong absorption. By comparative study of one-on-one wrapping and one-to-many encapsulation with geometrical selection of different MNSs, we found that the one-on-one wrapping model protected weakly-bonded nanogels from combination-induced distortion and strengthened nanogel networks via endowing exoskeleton. Besides, wrapping pattern and size-match significantly enhanced the quenching efficiency of MNSs towards the emissive nanogels. More importantly, the well-wrapped nanocomposites had considerable enhanced biological compatibility with much lower cytotoxicity and higher transfection capacity than the untailored MNSs composite and could serve as cellular glutathione detection.