Energy shortage and global warming are two grand challenges to human beings in the 21st century. The development of clean alternative energies and emission control of gases, such as CO 2 , have become most-urgent research fields. For the development of clean alternative energies, a wide range of approaches has been explored, including solar cells, [1] fuel cells, [2] and thermoelectric devices.[3] Solar cells, fuel cells, and thermoelectric devices convert optical, chemical, and thermal energies to electrical energy, respectively. Generation of electric energy from conversion of mechanical energy is of great interest owing to its abundance and unique fit for some applications. Recently, ZnO-nanowire (NW)-array-based piezoelectric nanogenerators have been demonstrated to convert mechanical energy to electricity by utilizing the coupling effect of the semiconducting and piezoelectric properties of ZnO. [4][5][6] Further exploration of this piezotronic concept [7] has led to the development of a wide variety of ZnO-NW-based piezotronic devices, such as piezoelectric field effect transistors, [8] nanoforce sensors, [8] and gate diodes.[9]More recently, CdS NWs were also successfully demonstrated for piezoelectric nanogenerators.[10] As another member in the wurtzite family, CdS is a piezoelectric, semiconducting, [11] and optoelectric [12] material with a direct energy band gap of about 2.5 eV [13] (corresponding to an on-set absorption of 500 nm). A wide range of 1D CdS nanostructures such as NWs, [14] NW arrays, [15] nanobelts, [16] nanotubes, [17] nanocombs, [18] and tetrapods, [19] have been synthesized by wet-chemistry or vapor-phase processes. The photon-induced conduction of 1D CdS nanostructures has also been demonstrated and studied. [20] A wide variety of 1D CdS nanostructure-based optoelectronic devices, such as photoconductors, [20] waveguides, [21] lasers, [22] logic gates, [23] field emitters, [24] and field-effect transistors (FETs) [25,26] have been developed.