The Collaborative International Dictionary of English v.0.48:

Great-hearted \Great"-heart`ed\, a.
   1. High-spirited; fearless. [Obs.] --Clarendon.
      [1913 Webster]

   2. Generous; magnanimous; noble. [WordNet sense 1]
      [1913 Webster]

Moby Thesaurus II by Grady Ward, 1.0:

78 Moby Thesaurus words for "greathearted":
   almsgiving, altruistic, beneficent, benevolent, big, bighearted,
   bold, bold-spirited, bounteous, bountiful, brave, charitable,
   chivalric, chivalrous, considerate, courageous, doughty,
   eleemosynary, elevated, exalted, fearless, free, freehanded,
   freehearted, gallant, generous, giving, gracious, great,
   great of heart, handsome, hardy, heroic, herolike, high,
   high-minded, hospitable, humanitarian, idealistic, intrepid,
   ironhearted, knightlike, knightly, large, largehearted, lavish,
   liberal, lionhearted, lofty, magnanimous, manful, manly,
   munificent, noble, noble-minded, open, openhanded, openhearted,
   philanthropic, princely, profuse, soldierlike, soldierly, stalwart,
   stintless, stout, stouthearted, sublime, ungrudging, unselfish,
   unsparing, unstinted, unstinting, valiant, valorous, welfare,
   welfare statist, welfarist