One-dimensional nanostructures, including nanotubes, nanowires, and nanorods, are potentially ideal functional components for nanometer-scale electronics and optoelectronics. However, the ability to fabricate nanoscale heterostructures with well-defined crystalline interfaces opens up many new device applications, as already proven in thin-film semiconductor electronics and photonics. This paper reports the catalyst-free fabrication of quantum-well nanorod heterostructures that exhibit atomically abrupt interfaces and a well-width dependent blue shift resulting from quantum confinement.