Consistent evidence shows that the cooperative and disparate relaxation of the segmental length, energy, vibration frequency, and polarization stimulated by molecular undercoordination results in skin supersolidity dictate the performance and functionality of core-shell configurated water droplets, in terms of the extraordinary chemical reactivity, catalytic capability, elastic adaptivity, hydrophobicity, hydro-voltaicity, sensitivity, thermal stability, and so forth. Understanding from the perspective of bonding and electronic dynamics could impact on engineering water droplets beneficial to scientific progress and life quality of human beings.