Owing to the boom of smartphone industries, the expansion of phone users has also been significant. Besides adults, children and elders have also begun to join the population of daily smartphone users. Such an expansion indeed facilitates the further exploration of the versatility and flexibility of digitization. However, these new users may also be susceptible to issues such as addiction, fraud, and insufficient accessibility. To fully utilize the capability of mobile devices without breaching personal privacy, we build the first corpus for age group recognition on smartphones with more than 1,445,087 unrestricted actions from 2,100 subjects. Then a series of heuristically-selected and neurally-guided features are proposed to increase the separability of the above dataset. Finally, we develop AgeCare, the first implicit and continuous system incorporated with bottom-to-top functionality without any restriction on user-phone interaction scenarios, for accurate age group recognition and age-tailored assistance on smartphones. Our system performs impressively well on this dataset and significantly surpasses the state-of-the-art methods.