The reliable, high-sensitive, wireless, and affordable requirements for humidity sensors are needed in high-precision measurement fields. Quartz crystal microbalance (QCM) based on the piezoelectric effect can accurately detect the mass changes at the nanogram level. However, water-capture materials deposited on the surface of QCM generally show disadvantages in either cost, sensitivity, or recyclability. Herein, novel QCM-based humidity sensors (NQHSs) are developed by uniformly depositing green microspheres (GMs) of natural polymers prepared by the chemical synthesis of the emulsification/inner gel method on QCM as humidity-sensitive materials. The NQHSs demonstrate high accuracy and sensitivity (27.1 Hz/% RH) owing to the various hydrophilic groups and porous nano-3D deposition structure. Compared with the devices deposited with a smooth film, the frequency of the NQHSs shows almost no changes during the cyclic test and exhibits long-term stability. The NQHSs have been successfully applied to non-contact sensing human activities and remote real-time humidity monitoring via Bluetooth transmission. In addition, the deposited humidity-sensitive GMs and QCM substrate are fully recycled and reused (72% of the original value). This work has provided an innovative idea to construct environmental-friendly, high-sensitivity, and wireless humidity sensors.