and eye-like digital cameras [15,16] ) with biological tissues without mechanically induced irritation. [17][18][19][20] A challenge of the flexible and stretchable electronics is to accommodate large deformations of biological tissues. [7,[21][22][23] One of the solutions to address this challenge involves the development of organic semiconductor materials that have high fracture strains. [24][25][26] Alternatives rely on structure designs to achieve high stretchability, [27][28][29][30] such as the integration of serpentine interconnects and inorganic functional materials with a soft elastomeric substrate. [31][32][33][34][35] A disadvantage of such integrated system is that the serpentine interconnects are bonded to the elastomeric substrate, which constraints the free buckling of the serpentine interconnects and therefore limits the stretchability of the devices. [36][37][38] Many designs were proposed to reduce the constraints of the elastomeric substrate on the serpentine interconnect to improve the stretchability, e.g., microfluidic assemblies, [21,39] core/shell packages, [40] and patterned substrate. [41,42] The preparation process of the patterned substrate is the simplest among these approaches. However, the major challenge to exploit patterned substrates is to precisely position the serpentine interconnects on the patterned substrates. The stretchability of the integrated systems depends on the alignment and position between the serpentine interconnects and patterned substrates, which has great randomness. [43] In this paper, an integrated system combining serpentine interconnects with toothed substrates is proposed to improve the stretchability of the serpentine interconnects bonded to conventional planar substrates. Here, the straight segments of the serpentine interconnects are bonded to the teeth molds of the toothed substrates as shown in Figure 1e. The arc segments (maximum strain area) of the serpentine interconnects are freestanding in this design so that it can provide high stretchability for the system. Furthermore, slight translation between the serpentine interconnects and toothed substrates changes little of the freestanding dimension of the arc segments. Therefore, such an integrated system also solves the challenge of uncontrolled stretchability for traditional patterned substrates. Systematic studies include results from quantitative experiments and comparisons with analytical models and finite element method computations. These studies have general utility for future work on stretchability design for flexible and stretchable electronics.Integration of deformable serpentine interconnects and inorganic functional materials with soft elastomeric substrate enables the electronics to deform into arbitrary desired shapes. Conventionally, the serpentine interconnects are bonded to a planar substrate, which limits the out-of-plane buckling of the serpentine interconnects, and thus restricts their stretchability. An integrated system combining serpentine interconnects with toothed substrate is...