Quick progress in the field of smart wearable devices requires self-sustainable power systems to help the devices execute the desired functions within a sufficient time scale. Because these devices have started to become small, light, compliant, complex, and multifunctional, it is challenging to provide them with the large amounts of energy necessary for their operation. Thus, future multifunctional wearable devices should not only incorporate mechanical flexibility for conformal contacts but also include sustainable energy units for stable operation. Hence, strategies for designing the assembly of nanoscale materials in macroscale-structured devices have attracted intense interest, with an aim to achieve mechanically deformable and sustainable wearable devices while exploiting the recent advances in nanomaterials and device fabrication. This review highlights the recent progress in nanomaterialenabled and structured energy harvesting, energy storage, and hybrid devices for powering sustainable wearables. In particular, one summarizes describe biomechanical energy harvesters (piezoelectric nanogenerators and triboelectric nanogenerators), solar energy harvesters (solar cells), biothermal energy harvesters (thermoelectric nanogenerators), energy storage devices (batteries and supercapacitors), and hybrid devices and focus on the use of nanomaterials and device configurations in 1D, 2D, and 3D structures, with an aim to shape the future demand for self-sustainable wearables.