With the recent development of in situ transmission electron microscopy (TEM) characterization techniques, the real time study of property-structure correlations in nanomaterials becomes possible. This dissertation reports the direct observations of deformation behavior of Al2O3-ZrO2-MgAl2O4 (AZM) bulk ceramic nanocomposites, strengthening mechanism of twins in YBa2Cu3O7-x (YBCO) thin film, work hardening event in nanocrystalline nickel and deformation of 2wt% Al doped ZnO (AZO) thin film with nanorod structures using the in situ TEM nanoindentation tool. The combined in situ movies with quantitative loading-unloading curves reveal the deformation mechanism of the above nanomaterial systems. At room temperature, in situ dynamic deformation studies show that the AZM nanocomposites undergo the deformation mainly through the grain-boundary sliding and rotation of small grains, i.e., ZrO2 grains, and some of the large grains, i.e., MgAl2O4 grains. We observed both plastic and elastic deformations in different sample regions in these multi-phase ceramic nanocomposites at room temperature. Both ex situ (conventional) and in situ nanoindentation were conducted to reveal the deformation of YBCO films from the directions perpendicular and parallel to the twin interfaces. Hardness measured perpendicular to twin interfaces is ~50% and 40% higher than that measured parallel to twin interfaces, by ex situ and in situ, respectively. By using an in situ nanoindentation tool inside TEM, dynamic work hardening event in nanocrystalline nickel was directly observed. During stain hardening stage, abundant Lomer-Cottrell (L-C) locks formed both within nanograins and against twin boundaries. Two major mechanisms were identified during interactions between L-C locks and twin boundaries. Quantitative nanoindentation experiments recorded during in situ experiments show an increase of yield strength from 1.64 to 2.29 GPa during multiple loading-unloading cycles. In situ TEM nanoindentation has been conducted to explore the size dependent deformation behavior of two different types (type I: ~ 0.51 of width/length ratio and type II: ~ 088 ratio) of AZO nanorods. During the indentation on type I nanord structure, annihilation of defects has been observed which is caused by limitation of the defect activities by relatively small size of the width. On the other hand, type II nanorod shows dislocation activities which enhanced the grain rotation under the external force applied on more isotropic direction through type II nanorod.