The osmotic heat engine (OHE) is a promising technology for converting low grade heat to electricity. Most of the existing studies have focused on thermolytic salt systems. Herein, for the first time, we proposed to use thermally responsive ionic liquids (TRIL) that have either an upper critical solution temperature (UCST) or lower critical solution temperature (LCST) type of phase behavior as novel thermolytic osmotic agents. Closed-loop TRIL-OHEs were designed based on these unique phase behaviors to convert low grade heat to work or electricity. Experimental studies using two UCST-type TRILs, protonated betaine bis(trifluoromethyl sulfonyl)imide ([Hbet][Tf2N]) and choline bis(trifluoromethylsulfonyl)imide ([Choline][Tf2N]) showed that (1) the specific energy of the TRIL-OHE system could reach as high as 4.0 times that of the seawater and river water system, (2) the power density measured from a commercial FO membrane reached up to 2.3 W/m2, and (3) the overall energy efficiency reached up to 2.6% or 18% of the Carnot efficiency at no heat recovery and up to 10.5% or 71% of the Carnet efficiency at 70% heat recovery. All of these results clearly demonstrated the great potential of using TRILs as novel osmotic agents to design high efficient OHEs for recovery of low grade thermal energy to work or electricity.