Bycatch from the experimental longline operations in the Lakshadweep Sea were studied. The experiments were conducted on converted Pablo boats, originally used for pole and line fishing operations, to capture skipjack tuna in the Lakshadweep Islands. The overall bycatch rate was very high, with a mean hooking rate of 8.05/1000 hooks compared to the targeted tuna catch (1.75/1000 hooks). Bycatch contributed 82.4% of the catch in comparison to the tuna (17.6%) Thunnus albacares, in the longline operations. Silky shark (Carcharhinus falciformes) with 89.9% was the dominant shark species followed by C. amblyrhynchos, Galeocerdo cuvier, Alopias pelagicus, Negapriion acutedens and Sphyrna lewinii with 4.7, 2.7, 1.4, 0.7 and 0.7%, respectively. Sharks contributed to 74.1% of the catch, followed by 15.7% sailfishes and 10.2% miscellaneous fishes. Higher bycatch rates were evident during evening hours compared to mornings, but the results were not significant statistically. Studies on the effects of depth on the overall fishing performance and species selectivity failed to establish any significant relationship at a depth range of 35–100 m. Soaking time had a significant effect on bycatch rates. The hooking rate of sharks declined with an increase in soaking time. Considering the high shark bycatch in the fishery, an accurate monitoring of the longline fish catches in the Lakshadweep waters is an important step towards ensuring the sustainability of other populations, especially sharks.