Multifunctional wearable sensors have gained significant popularity in recent years for point of care diagnosis, tackling the myriad of obstacles faced in coping with health-related issues. However, complex fabrication, lack of biocompatibility, non-reusability, and accuracy limit their widespread use. In this work, we report a clean-room-free fabrication of molybdenum diselenide (MoSe2) interspersed with polyvinyl alcohol (PVA) based multifunctional device for in situ and non-invasive high-fidelity human gesture recognition, pulse rate monitoring, and skin hydration sensing. Detailed morphological characterization studies reveal the formation of a rhombohedral structure for MoSe2 nanoflakes stacked vertically to form a micro flower structure. Group synaptic activity of neurons results in a subtle electrical impulse, which, in turn, generates an electric field that is detected by the as-fabricated MoSe2/PVA device when attached to the forehead and interfaced to Open Brain-Computer Interface platform-based Cyton biosensing board. The device is also used as an ultrasensitive pressure sensor for arterial pulse pressure monitoring. This detection mechanism of the multifunctional sensor can be attributed to the piezoresistive effect of MoSe2 nanoparticles, wherein the dipoles reorient to form an internal polarization upon detection of physiological information. The strategy employed here paves the way toward replacing wet electrodes in conventional electroencephalogram (EEG)/electrocardiogram (ECG) measurements that result in skin abrasion and signal quality degradation with low-cost, reliable, skin-friendly, wearable MoSe2/PVA dry electrodes for rapid assessment. © 2022 Author(s).