Correlations between phase transition temperatures (Tpt) in aqueous solutions and quantitative amphiphilic characteristics of a large array of thermoresponsive molecular bottlebrushes, polymethacrylates containing oligoethylene glycol (OEG), oligopropylene glycol (OPG), higher n-alkyl blocks of different lengths in their side chains, have been systematically studied for the first time. The estimated hydrophilic-lipophilic balance (HLBp) of the polymers calculated from the HLBm of the starting monomers using the Davis group number method was used for the amphiphilic characterization. The adequacy of this approach was confirmed by analyzing experimental data on the distribution of monomers and polymers in hexane-water heterophase system. Depending on the mutual arrangement of OEG-, OPG- and n-alkyl blocks in macromolecules, 107 considered molecular brushes considered were divided into 5 types and specific correlations between Tpt and HLBp values were determined for each type. The correlations found can be used to predict the phase transition temperatures of promising thermoresponsive polymethacrylic molecular brushes containing OEG-, OPG- and higher n-alkyl blocks in the side chains when varying the length of the blocks and their ratio in the macromolecules.