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3-D integration provides a promising approach for the construction of complex microsystems through the bonding and interconnection of individually optimized device layers without sacrificing system performance. The use of traditional underfill processes is expected to face an arduous challenge as the filled gap of a large-scale chip is narrowed down to several micrometers. Consequently, the subsequent reliability of microbumps (μ-bumps) joints and the relative assembly compatibility of stacked chips of 3-D IC packages deteriorate. To resolve this critical issue, a novel technology for wafer-level underfill film (WLUF) is developed. This paper demonstrates the steps that the proposed technology would take. These steps include the alignment of the WLUF-coated chip to the substrate chip and the elimination of voids to make the proposed technology work. However, the coplanarity of stacked thin chips after assembling with the WLUF, is an urgent problem that needs to be understood in detail. Therefore, this paper presents a nonlinear finite element analysis (FEA) using a process-oriented simulation technique to estimate the warpage of stacked thin chips. For experimental validation, the effects of several key designed factors on the thermomechanical behavior of chip-on-chip package under various bonding forces are investigated. The analytic results indicate that a chip thickness of <; 50 μm at the outermost region of the packaging structure without μ-bumps significantly reduces approximately 2 μm of gap between chips. This phenomenon is attributed to the major structural support at the purlieus of the chip via WLUF, which is extremely weak when a uniform bonding pressure is loaded. In addition, the subsequent cooling procedure of the WLUF further aggravates the warpage magnitude of the stacked thin chips. The results of this paper could serve as a guideline for further improvement of the bonding reliability and for the design of the st- uctural optimization of packaging assemblies via the WLUF.