No-flow underfill materials that cure during the solder reflow process is a relatively new technology. Although there are several advantages in terms of cost, time and processing ease, there are several reliability challenges associated with no-flow underfills. When micron-sized filler particles are introduced in no-flow underfills to enhance the solder bump reliability, such filler particles could prevent the solder bumps making reliable electrical contacts with the substrate pads during solder reflow, and therefore, the assembly yield would be adversely affected. The use of nano-sized filler particles can potentially improve assembly yield while offering the advantages associated with filled underfill materials. The objective of this thesis is to study the thermo-mechanical reliability of nano-filled epoxy underfills (NFU) through experiments and theoretical modeling. In this work, the thermo-mechanical properties of NFUs with 20-nm filler particles have been measured. An innovative residual stress test method has been developed to measure the interfacial fracture toughness. Using the developed residual stress method and the single-leg bending test, the mode-mixity-dependent fracture toughness for NFU-SiN interface has been determined. In addition to such monotonic interfacial fracture characterization, the interface crack propagation under thermo-mechanical fatigue loading has been experimentally characterized, and a model for fatigue interface crack propagation has been developed. A test vehicle comprising of several flip chips was assembled using the NFU material and the reliability of the flip-chip assemblies was assessed under thermal shock cycles between -40oC and 125oC. The NFU-SiN interfacial delamination propagation and the solder bump reliability were monitored. In parallel, numerical models were developed to study the interfacial delamination propagation in the flip chip assembly using conventional interfacial fracture mechanics as well as cohesive zone modeling. Predictions for interfacial delamination propagation using the two approaches have been compared. Based on the theoretical models and the experimental data, guidelines for design of NFUs against interfacial delamination have been developed.