The effects of time (10–60 min) and temperature (250–350°C) on TOCcrude and biochar yields from coir and pith through hydrothermal liquefaction (HTL) process was investigated. The parameters were optimized for minimum biochar and maximum total organic carbon (TOC) in aqueous crude using response surface methodology (RSM). The optimal time and temperature for HTL of coir and pith were 35 min, 302°C, and 35.2 min, 300°C, respectively. Higher biomass conversion and bio-oil yield of 87.34%, 83.76% and 34.6%, 32.72%, was observed for coir and pith, respectively. The biochar yield for coir and pith was reduced from 40 to 12.66% and 34–16.24%. The oxygen and carbon content in the HTL products such as heavy bio-oil (HBO), light bio-oil (LBO) were lower and higher increasing the High Heating Value (HHV), respectively. The HHV of HBO, and LBO for coir and pith were 31 MJ/kg, 22 MJ/kg and 28 MJ/kg, 19 MJ/kg, respectively. The GC-MS/MS analysis revealed that the oil was a mixture of compounds such as alcohols, aldehydes, ketones, amines, amides, esters, ethers, phenols, and their derivatives. Therefore, the conversion of coir and pith to bio-oil can be effectively achieved through the HTL process. © 2021