specific surface area. [1,2] The nontrivial band structure of graphene near the Fermi level enables a series of appealing phenomena, e.g., the anomalous quantum Hall effect, [3] ultrahigh electron mobility, [4] and superior thermal conductivity, [5] rendering it a promising candidate for the next generation of micro/nanoelectronic devices. With respect to its current status and future perspectives, it is of great significance to fully explore the tunability of the properties of graphene by various methods, e.g., doping, [6] gating, [7] and strain engineering. [8,9] Among these approaches, strain engineering is capable of altering the lattice symmetry of graphene, thus tuning its electronic band structure, [10,11] which could be superior in the bandgap opening, [12] conductance modulation, [13,14] and the formation of strong magnetic field. [15] For a realistic graphene-integrated optoelectronic device in an on-chip manner, such as optical modulators, [16] silicongraphene photodetectors, [17,18] and broadband polarizer, [19] strain engineering is desired in order to provide a flexible approach for tuning the electrical structure of graphene. However, developed strain-tuning methods, such as the deformation of flexible substrates, [20,21] piezoelectric substrate actuation, [22] and pressurized blisters, [23] are hardly compatible with onchip applications. Particularly, using the rolling method as a reliable approach for both optimal yields and effective strain manipulation [24][25][26] suggests direct and precise tuning with target morphologies and thus their mechanical properties. [27] Based on rolling geometry, the corresponding strain states in graphene can be designed and accurately realized, as summarized in Figure 1, where the tensile strain in graphene could be introduced through the transfer process of graphene onto conventional semiconductors. [28,29] However, compressive strain in graphene is seldom reported because the critical compressive strain for buckling is several orders of magnitude smaller than the critical tensile strain for fracturing. [30] Furthermore, for a few compressive strain cases, it is essential to explore the fundamental physics of out-of-plane deformation, which often occurs during the compression process.On the other hand, the innovative 3D architecture based on 2D graphene and graphene oxide enables morphologyengineered performance, such as strong mechanical properties, On-chip strain engineering is highly demanded in 2D materials as an effective route for tuning their extraordinary properties and integrating consistent functionalities toward various applications. Herein, rolling technique is proposed for strain engineering in monolayer graphene grown on a germanium substrate, where compressive or tensile strain could be acquired, depending on the designed layer stressors. Unusual compressive strains up to 0.30% are achieved in the rolled-up graphene tubular structures. The subsequent phonon hardening under compressive loading is observed through straininduced Raman G band splittin...