Simply end the paragraph before closing the group associated to \Large so the corresponding \baselineskip will be applied; you can do this by adding \par:
\documentclass{article}
\begin{document}
\begin{center}
\Large\textbf{The Great Thesis About Some Very Great Things Indeed With
a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So}
\end{center}
\begin{center}
\Large\textbf{The Great Thesis About Some Very Great Things Indeed With
a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So}\par
\end{center}
\end{document}
Here's a comparison of both results:

I removed the outer braces since they are not necessary, as the center environment already forms a group.
If you want to have more control over the spacing, you could use the second argument of \fontsize (the first argument gives the font size); a little example:
\documentclass{article}
\begin{document}
\begin{center}
\fontsize{15pt}{15pt}\selectfont\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\begin{center}
\fontsize{15pt}{18pt}\selectfont\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\begin{center}
\fontsize{15pt}{30pt}\selectfont\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\end{document}
producing now:

Another option, not requiring you to explicitly know the font size, is to change the factor in the mandatory argument of \linespread:
\documentclass{article}
\begin{document}
\begin{center}
\linespread{1}\Large\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\begin{center}
\linespread{0.8}\Large\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\begin{center}
\linespread{2}\Large\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\end{document}

Yet another option is a redefinition of \baselinestretch; the following code will produce the same result illustrated just above:
\documentclass{article}
\begin{document}
\begin{center}
\renewcommand\baselinestretch{1}\Large\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\begin{center}
\renewcommand\baselinestretch{0.8}\Large\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\begin{center}
\renewcommand\baselinestretch{2}\Large\bfseries The Great Thesis About Some Very Great Things Indeed With a Pretty Long Title That Will Probably Be Split Between at Least Two Lines
Or So
\end{center}
\end{document}
Finally, there's the setspace package which offers you a series of commands and environments to change "in a sensible way" the value of \baselineskip.
setspacepackage that provides\singlespacing,\onehalfspacingand\doublespacingcommands. – Mar 21 '12 at 00:05setspace, be careful with this! Just by including the package (without using any commands of it), it destroyed the layout for me in some places. – letmaik May 27 '13 at 10:59\linespread{..}is used without changing font size/style afterwards, then a\selectfontmust follow. – letmaik May 27 '13 at 11:15