Although considerable accomplishments have been achieved, it remains a big challenge to prepare wearable strain sensors with high sensitivity and broad sensing range simultaneously. [3][4][5][6] To achieve a balance between high sensitivity and broad range, the effects of some factors like substrate stiffness and interfacial interactions between conductive nanomaterials and elastic polymers on the performance of strain sensors have been investigated. [7,8] Cao et al. prepared fiberbased strain sensors with different GF and work ranges by adjusting the bonding layer between silver nanowires and PU substrate. Specially, a wide work range of 0-50% and a large GF of 940 were both possessed for Ag NW/PU-9.2 wt%/5 min fiber. However, GF was still very small at low strain range (from 0.1 to 118 within 35% strain). [9] Recently, rational design of the geometric structure is considered as an effective strategy to solve the above dilemma between high sensitivity and broad workable range for strain sensors. Flexible strain sensors with novel microstructures, [10][11][12][13] including the crack structure, [14][15][16] the buckling structure, [17,18] the gradient structure [19][20][21] and the biomimetic hierarchical structure, [22] have been reported for fabricating highperformance strain sensors. Gao et al. prepared a multilayered fiber-based strain sensor with high sensitivity and broad workable range (GF = 166.7 at 350% strain) with a hollow-monolith microstructure through a coaxial wet-spun method. [23] To date, many wearable strain sensors based on graphene have been studied owing to its outstanding electrical, mechanical, and thermal properties. [24][25][26][27] Wang et al. developed a strain sensor based on reduced graphene oxide (RGO)-decorated PU electrospun mats, and GF = 11 at 10% strain and GF = 79 at 100% strain were obtained. [28] Cheng et al. presented a graphene-based fiber with a "compression spring" structure, which possessed a detection limit of 0.2% strain (GF = 10 within 1% strain) and broad workable range (100%). [29] However, the above studies always show low sensitivity (GF < 20), especially at low strain range, due to the slippage of graphene flakes. To increase the sensitivity of graphene-based sensor, different polymers have been used as "mortars" with graphene flakes as "bricks," including bovine serum albumin (BSA), [30] chitosan, [31] poly(vinyl alcohol), [32] and polyethylenimine (PEI). [33] However, the above polymers are always nonconductive, which It remains a challenge to achieve high sensitivity and a broad linear strain range simultaneously for wearable strain sensors. Specially, graphene-based strain sensors always exhibit low sensitivity owing to the slippage of graphene flakes. To overcome this problem, Al 3+ is used here as "mortars" for graphene flakes instead of polymers usually used in the literature, and thus a very simple and low-cost strategy is developed to prepare a high-performance reduced graphene oxide coated fiber strain sensor. The strain sensor shows a low detection lim...