Flexible interconnects are one of the key elements in realizing next-generation flexible electronics. While wire bonding interconnection materials are being deployed and discussed widely, adhesives to support flip-chip and surface-mount interconnections are less commonly used and reported. A polyurethane (PU)-based electrically conductive adhesive (ECA) is developed to meet all the requirements of flexible interconnects, including an ultralow bulk resistivity of approximate to 1.0 x 105 cm that is maintained during bending, rolling, and compressing, good adhesion to various flexible substrates, and facile processing. The PU-ECA enables various interconnection techniques in flexible and printed electronics: it can serve as a die-attach material for flip-chip, as vertical interconnect access (VIA)-filling and polymer bump materials for 3D integration, and as a conductive paste for wearable radio-frequency devices.