Anisotropic strain engineering has emerged as a powerful strategy for enhancing the optoelectronic performance of semiconductor nanocrystals. Here, we show that CdSe/CdS dot-in-rod structures offer a platform for fine-tuning the optical response of CdSe quantum dots through anisotropic strain. By controlling the spatial position of the CdSe core within a growing CdS nanorod shell, varying degrees of uniaxial strain can be introduced. Placing CdSe cores at the end of the CdS nanorod induces strong asymmetric compression along the c-axis of the wurtzite CdSe core, dramatically altering its absorption and emission characteristics, whereas CdSe cores located near the middle of the nanorod experience a comparatively weak uniaxial strain field. The change in absorption and emission spectra and dynamics for highly strained end-position CdSe/CdS nanorods is explained by (1) relative shifting of the valence band light hole and heavy hole levels and (2) introduction of a strong piezoelectric potential, which spatially separates the electron and hole wave functions. The ability to tune the degree of uniaxial strain through core position control in a nanorod structure creates opportunities for precisely modulating the electronic properties of CdSe nanocrystals while simultaneously taking advantage of dielectric and optical anisotropies intrinsic to 1D nanostructures.