Stretchable film strain sensors show potential applications in healthcare and human‐machine interfacing, while poor signal linearity restricts their practical applications owing to inaccurate and instable strain indication. Signal sensitivity and linearity can be improved via constructing hetero‐modulus microstructure on elastomeric substrate to some extent, though it is challenging to construct hetero‐structure with distinct modulus differences for electrical signal linearity modulation over a wide strain range. Herein, a simple strategy is proposed to tune signal sensitivity, linearity, and detection range of stretchable strain sensors by adjusting the distribution of rigid polystyrene (PS) nanospheres coated on electrospun thermoplastic polyurethane (TPU) fiber mats. Heterostructure characteristics can be controlled by spray coating times of PS nanospheres, which are immobilized onto the fiber mats by weak swelling of TPU and the linking layer of reduced graphene oxide (rGO) between TPU and PS induced by hydrogen bonding and π–π stacking. Relatively, the sensors with moderate spray coating times of PS nanospheres show balanced signal sensitivity and linearity over a strain range of 0–80%, as well as fast response to tensile strain and good signal reproducibility. Such elastomeric film strain sensors can be used for monitoring physiological activities and interfacing human hand and bionic fingers.