to motion sensors. [9][10][11][12][13][14][15][16][17] In particular, flexible thin-film strain sensors (FTSS) that are attached to epidermis and detect small movements have received intensive research interest. [11,[17][18][19][20][21][22] According to working mechanisms, FTSS devices can be categorized based on the employed capacitive, [17,19] piezoelectric, [23][24][25] piezoresistive, [11,18,26] and optical effects. [27][28][29] The materials range from stretchable polymers, such as poly(dimethyl siloxane) (PDMS) [11,26,[30][31][32] and Ecoflex, [33] to conductive fillers, such as nanowires, [34,35] nanoparticles, [21,36] and low dimensional carbonaceous materials, [10][11][12]18,33,37] as well as their hybrid micro-/nanostructures. [38][39][40] In particular, owing to the excellent mechanical compliancy and unique electric characteristics, substantial efforts have been focused on exploiting carbonaceous materials such as carbon nanotubes (CNTs) [11,18,33,39,[41][42][43][44][45][46][47][48][49][50][51][52] and graphene [9,10,30,31,40,51,[53][54][55][56][57][58][59][60][61] in the development of FTSS.Carbon nanotubes, a type of quasi-1D structures with high aspect ratios, have been developed in the formation of percolation conducting networks for elastic strain sensors. [22] The high elasticity in such sensors can be attributed to the homogeneous propagation of microcracks in CNT films and extendable lateral space among aligned CNTs. Both the pressure and tensile strain sensors made of CNTs that utilize the capacitive effect can sustain strains up to 300%. [18,41] The working principle of such sensors, however, limits the gauge factor (GF) up to 1, [22] where the GF is a parameter used to characterize the strain sensitivity of resistive strain sensors and is given by GF = (R − R 0 )/(R 0 ε) and ε is strain. By employing the piezoresistive mechanism, a class of wearable and stretchable devices fabricated from thin films of aligned single-walled carbon nanotubes on PDMS substrates can provide a large range of strains up to 410% and improved GF up to 12. [11,62] A GF as high as 35 can be achieved at a strain of 1%. [44] It can be found that the CNTbased strain sensors usually exhibit high tolerance in strains while low GFs. In contrast, the excellent piezoresistive properties of 3D graphene foams with monolithic porous structures allow strain sensors constructed from these materials offering much higher GFs. [22] Chen et al. fabricated 3D interconnected graphene networks using chemical vapor deposition (CVD) and embedded these networks in a PDMS matrix to create strain sensors that withstand tensile strains up to 95% and provide a GF of 2. [26] Graphene in nanocellulose nanopapers show aThe design and fabrication of various types of flexible, portable, and foldable devices have received immense interest owing to the remarkable potential in impacting peoples' lives including real-time health monitoring, pointof-care diagnosis, and athletic training. In this work, the authors present 3D graphite as the key sensing ...