'Grand'(adjective) means big, large, or huge. 'Hustle'(verb or noun) literally means to hurry or work harder. However, used in the urban connotation, hustle means to grind or to get something quickly. That something could be money or just anything one wants or needs. So, grand hustle is defined as being on a big mission to get what you want or need.
I'm on a grand hustle to get money for college.
Grand Hustle is an American record label formed by Clifford ("T.I.") Harris and Jason Geter in 2003. The label is being distributed by Asylum Records and Atlantic Records. The label includes artists TI, P$C, Young Dro, Governor, Big Kuntry, Xtaci, Alfamega, and Rashad.
Young Dro just released his debut album from Grand Hustle.