We designed and fabricated terminated polymer waveguides with low coupling loss to a standard single-mode fiber (SSMF) for 100 Gbps optical interconnects application and beyond. The mode field diameter of the polymer waveguide is designed to perfectly match that of the SSMF with a theoretical coupling loss as small as 0.07 dB. The fabricated polymer waveguides on FR-4 substrates exhibit both a low propagation loss of 0.32 dB/cm and a low coupling loss of less than 0.17 dB to SSMF at a wavelength of 1310 nm. These low loss values indicate good compatibilities with both printed circuit boards and fiber optics. Both single-lane 56 Gbaud (112 Gbps) and 60 Gbaud (120 Gbps) 4-level pulse amplitude modulation (PAM4) optical transmission using terminated polymer waveguides have been successfully demonstrated. The bit error ratio (BER) for PAM4 transmission at both data rates reached a level of 10−4 which is well below the forward error correction (FEC) limitation with a power penalty of less than 1 dB. The bandwidth of the test equipment rather than the polymer waveguide itself limits the high-speed optical interconnect performances in our experiments. The results imply that the polymer waveguide is a promising media for single-lane 100 Gbps optical interconnects application and beyond.