Hydrogel bioelectronics as one of the next-generation wearable and implantable electronics ensures excellent biocompatibility and softness to link the human body and electronics. However, volatile, opaque, and fragile features of hydrogels due to the sparse and microscale three-dimensional network seriously limit their practical applications. Here, we report a type of smart and robust nanofibrillar poly(vinyl alcohol) (PVA) organohydrogels fabricated via one-step physical cross-linking. The nanofibrillar network cross-linked by numerous PVA nanocrystallites enables the formation of organohydrogels with high transparency (90%), drying resistance, high toughness (3.2 MJ/m³), and tensile strength (1.4 MPa). For strain sensor application, the PVA ionic organohydrogel after soaking in NaCl solution shows excellent linear sensitivity (GF = 1.56, R² > 0.998) owing to the homogeneous nanofibrillar PVA network. We demonstrate the potential applications of the nanofibrillar PVA-based organohydrogel in smart contact lens and emotion recognition. Such a strategy paves an effective way to fabricate strong, tough, biocompatible, and ionically conductive organohydrogels, shedding light on multifunctional sensing applications in next-generation flexible bioelectronics.