The gelation of locust bean gum in concentrated sucrose solutions has been studied as a function of temperature, LBG and sucrose concentrations. A critical gelling concentration of approximately 1% w/w LBG in 60% w/w sucrose was measured. The gelation rate initially increased with decreasing temperature until a maximum in gelation rate was found close to -5 degrees C. Along with the large temperature hysteresis between the temperature for maximum gelation rate and the melting temperature (>44 degrees C), it is proposed that the cross-linking was controlled by nucleation and growth processes rather than reversible pairwise cross-linking. The slow evolution of LBG cross-links was detected at lower frequencies through an increase in the storage modulus, while at higher frequencies a decrease in the storage modulus was observed. This decrease at higher frequencies was associated with a reduction in chain entanglements during the initial stages of gelation. In addition to cross-link formation through association of 1,4-linked p-D-mannan regions which were sterically uninhibited by galactose, chain localization may also have been entropically driven due to a reduction in solvent quality as the temperature was decreased toward the gelling temperature. LBG exhibited incompatible behaviour at high sucrose concentrations as a rheological inversion was detected for sucrose concentrations greater than 50% w/w sucrose (at 1.5% w/w LBG), where the polymer rheology changed to that resembling a concentrated sucrose solution. A rheological assessment of the influence of temperature upon the viscoelastic properties of a concentrated LBG/sucrose solution was also performed using the time/temperature superposition principle. The evaluated WLF constants c(1) and c(2) were 7.5 and 50 K for T-g=255 K, similar to those reported for sucrose, glucose, and maltodextrin solutions and several inorganic and organic liquids. These constants did not retain their original meaning, however, owing to the heterogeneous nature of 1.5% w/w LBG, 60% w/w sucrose solution, as reflected by the theologically derived high glass transition temperature.