Carbon nanotube (CNT) forests are an important class of nanomaterials with many potential applications due to their unique properties such as mechanical compliance, thermal and electrical conductance, etc. Their deformation and failure in compression loading is critical in any application involving contact because the deformation changes the nature of the contact and thus impacts the transfer of load, heat, and charge carriers across the interface. The micro- and nano-structure of the CNT forest can vary along their height and from sample to sample due to different growth parameters. The morphology of CNTs and their interaction contribute to their mechanical behavior with change of load distribution in the CNT forest. However, the relationship is complicated due to involvement of many factors such as density, orientation, and entanglement of CNTs. None of these effects, however, are well understood. This dissertation aims to advance the knowledge of the structure-property relation in CNT forests and find methodologies for tuning their mechanical behavior. The mechanical behavior of CNT forests grown with different methodologies is studied. Furthermore, the effects of coating and wetting of CNT forests are investigated as methods to tailor the degree of interaction between CNTs. In situ micro-indentation of uncoated CNT forests with distinct growth-induced structures are performed to elucidate the effects of change of morphology along the height of CNT forests on their deformation mechanism. CNT aerial density and tortuosity are found to dictate the location of incipient deformation along height of CNT forests. Macro-compression testing of uncoated CNT forests reveals mechanical failure of CNT forests by delamination at the CNT-growth substrate. Tensile loading of CNT roots due to post-buckling bending of CNTs is proposed to be the cause of this failure and simple bending theory is shown to estimate the failure load to be on the same order of magnitude as experimental measurements. Furthermore, delamination is observed to occur in the in situ micro-indentation of CNT forests coated with aluminum on the top surface, which demonstrates the role of the mechanical constraints within the CNT forest in the occurrence of delamination at the CNT-substrate interface. In addition, this dissertation explores the mechanical behavior of CNT forests coated conformally (from top to bottom) with alumina by atomic layer deposition. In situ micro-indentation testing demonstrates that the deformation mechanism of CNT forests does not change with a thin coating (2 nm) but does change with a sufficiently thick coating (10 nm) that causes fracturing of the hybrid nanotubes. Ex situ flat punch and Berkovich indentations reveal an increase in stiffness of the CNT forests that are in range with those predicted by compression and bending theories. An increase in the recoverability of the CNTs is also detected. Finally, solvent infiltration is proposed as a method of decreasing stiffness of CNT forests and changing the deformation mechanism from local to global deformations (i.e., buckling in the entire height). Presence of solvents between CNTs decreases the van der Waals forces between them and produces CNT forests with lower stiffness. The results demonstrate the effect of interaction between CNTs on the mechanical behavior. This dissertation reveals important information on the mechanical behavior of CNT forests as it relates to CNT morphology and tube-to-tube interactions. In addition, it provides a framework for future systematic experimental and theoretical investigations of the structure-property relationship in CNT forests, as well as a framework for tuning the properties of CNT forests for diverse applications.