First of all, the commas. A comma means that the text of the node is ended, and options pertaining to it follows. To have commas in the node text, wrap it in braces.
Second, \left/\right. They require math mode, and they also require a delimiter to follow them, which you've forgotten. I'd remove them altogether though, and insert just (/) instead. \left .. \right isn't needed when you only have numbers between them like that.
As noted in a comment below, align=center doesn't really do much useful here, so unless you're planning to, for example, add linebreaks, it can be removed.
\documentclass[tikz,border=10pt]{standalone}
\usepackage{forest}
\begin{document}
\begin{forest}
for tree={
draw
}
[{TowersOfHanoi(4, 1, 3, 2)}
[{TowersOfHanoi(3, 1, 2, 3)}
[{TowersOfHanoi(2, 1, 3, 2)}
[{TowersOfHanoi(1, 1, 2, 3)}]
[{TowersOfHanoi(1, 2, 3, 1)}]
]
[{TowersOfHanoi(2, 3, 2, 1)}
[{TowersOfHanoi(1, 3, 1, 2)}]
[{TowersOfHanoi(1, 1, 2, 3)}]
]
]
[{TowersOfHanoi(3, 2, 3, 1)}
[{TowersOfHanoi(2, 2, 1, 3)}
[{TowersOfHanoi(1, 2, 3, 1)}]
[{TowersOfHanoi(1 ,3, 1, 2)}]
]
[{TowersOfHanoi(2, 1, 2, 2)}
[{TowersOfHanoi(1, 1, 2, 3)}]
[{TowersOfHanoi(1, 2, 3, 1)}]
]
]
]
\end{forest}
\end{document}
That said, your tree becomes very wide when you write TowersOfHanoi in every node. Perhaps you could consider abbreviating it to ToH, or leaving it out altogether.
\documentclass[tikz,border=10pt]{standalone}
\usepackage{forest}
\begin{document}
\begin{forest}
for tree={
draw,
}
[{ToH(4, 1, 3, 2)},label={above:ToH = TowersOfHanoi}
[{ToH(3, 1, 2, 3)}
[{ToH(2, 1, 3, 2)}
[{ToH(1, 1, 2, 3)}]
[{ToH(1, 2, 3, 1)}]
]
[{ToH(2, 3, 2, 1)}
[{ToH(1, 3, 1, 2)}]
[{ToH(1, 1, 2, 3)}]
]
]
[{ToH(3, 2, 3,1)}
[{ToH(2, 2, 1, 3)}
[{ToH(1, 2, 3, 1)}]
[{ToH(1, 3, 1, 2)}]
]
[{ToH(2, 1, 2, 2)}
[{ToH(1, 1, 2, 3)}]
[{ToH(1, 2, 3, 1)}]
]
]
]
\end{forest}
\begin{forest}
for tree={
draw,
}
[{(4, 1, 3, 2)},label={above:Arguments to TowersOfHanoi}
[{(3, 1, 2, 3)}
[{(2, 1, 3, 2)}
[{(1, 1, 2, 3)}]
[{(1, 2, 3, 1)}]
]
[{(2, 3, 2, 1)}
[{(1, 3, 1, 2)}]
[{(1, 1, 2, 3)}]
]
]
[{(3, 2, 3,1)}
[{(2, 2, 1, 3)}
[{(1, 2, 3, 1)}]
[{(1, 3, 1, 2)}]
]
[{(2, 1, 2, 2)}
[{(1, 1, 2, 3)}]
[{(1, 2, 3, 1)}]
]
]
]
\end{forest}
\end{document}
align=centerisn't doing much either. (It is adding a little vertical padding.) – cfr Sep 06 '17 at 02:52