Realization of sensing multidirectional strains is essential to understanding the nature of complex motions. Traditional uniaxial strain sensors lack the capability to detect motions working in different directions, limiting their applications in unconventional sensing technology areas, like sophisticated human-machine interface and real-time monitoring of dynamic body movements. Herein, a stretchable multidirectional strain sensor is developed using highly aligned, anisotropic carbon nanofiber (ACNF) films via a facile, low-cost, and scalable electrospinning approach. The fabricated strain sensor exhibits semitransparency, good stretchability of over 30%, outstanding durability for over 2500 cycles, and remarkable anisotropic strain sensing performance with maximum gauge factors of 180 and 0.3 for loads applied parallel and perpendicular to fiber alignment, respectively. Cross-plied ACNF strain sensors are fabricated by orthogonally stacking two singlelayer ACNFs, which present a unique capability to distinguish the directions and magnitudes of strains with a remarkable selectivity of 3.84, highest among all stretchable multidirectional strain sensors reported so far. Their unconventional applications are demonstrated by detecting multi-degrees-offreedom synovial joint movements of the human body and monitoring wrist movements for systematic improvement of golf performance. The potential applications of novel multidirectional sensors reported here may shed new light into future development of next-generation soft, flexible electronics.To satisfy the growing interests, significant efforts have been made to improve their overall performances. Various materials and structures, [14][15][16][17][18] including nanosize metals, [19][20][21][22] conductive polymers, [23][24][25] nanocarbon materials, [26][27][28][29][30] and fiber or core-shell structure, [14,16,31] have been utilized to enhance the sensitivity, stretchability, linearity, and stability. Unfortunately, however, these strain sensors are designed to mainly detect a uniaxial strain while sensing multidirectional strains has rarely been accomplished, restricting their widespread applications. [32,33] The difficulty in achieving multidirectional strain sensing is due to the macro-or microscopically isotropic nature of conducting networks of strain sensors, which usually experience similar deformation upon stretching in any direction. To address this issue, geometrically engineered flexible strain gauge rosettes [34] and cross-shaped strain sensors [35] composed of isotropic piezoresistive materials were introduced previously. However, they showed a limited success with a small sensing range and an insufficient capability to distinguish the changes in multiaxial strain conditions because the isotropic piezoresistive materials experience significant destruction in their networks at high strains, regardless of the loading directions. To measure complex motions in 3D space with high accuracy requires rational design and use of suitable materials capable of detect...