Future applications of flexible displays and wearable electronics will need 3-D stacked flexible interconnects. The interconnection of an ultrathin chip-on-flex (UTCOF) that can provide flexibility is one approach that meets this requirement. Therefore, thermally induced warpage of UTCOF interconnects using anisotropic conductive adhesive (ACA) is investigated. In this paper, the effects of the ACA joint material properties, bonding temperature, and chip thickness on warpage of ACA-bonded UTCOF interconnects are examined experimentally and numerically. Two film types of ACA materials, ACA-P and ACA-F, are assembled under different bonding temperatures to study the effects of bonding temperature on warpage via out-of-plane deformation measurements using a micro figure measurement instrument. Micro Au-bump and compliant-bump assemblies in 80-μm-pitch dummy test vehicles are evaluated. Moreover, ultrathin chips with 25-50 μm thickness were assembled onto polyimide flex substrates to study the effects of chip thickness on thermally induced warpage. The 85°C/85% relative humidity thermal humidity storage test (RH THST) was also conducted for 1000 h for the UTCOF assembled with the selected process parameters. The interfaces between the ultrathin silicon chip and substrate are inspected in cross-sectional scanning electron microscopy (SEM) images. To validate the results of the experiments, a rigorous 3-D finite element (FE) analysis model integrating both thermal and thermal-mechanical behaviors of the UTCOF is established and performed using the ANSYS program. Experimental and numerical results indicate that the warpage of the micro compliant-bump assembly is less than that of the micro Au bump. Furthermore, the averaged warpage of the ACA-P-bonded samples with the Au bump using a 50- μm-thick chip is around 50.3 μm at a bonding temperature of 160°C whereas that of the ACA-F-bonded samples is 64.4 μm at 190°C. Additionally, both thermal expansion mismatch and the thermal gradient between the ultrathin silicon chip and substrate strongly affect the thermal-mechanical behaviors of the UTCOF interconnects. As expected, warpage increases as thickness of an ultrathin silicon chip decreases. A strong correlation exists between FE analysis results and experimental results. The manufacturing technology for high-density and flexible UTCOF interconnects with ACA joints is thus established.