This thesis is concerned with unsupervised learning of syntactic structure from plain text corpora by aligning sentences. Based on Harris (1951) linguistic notion of substitutability, sentences in a plain text corpus can be compared to each other and those parts that have similar context and in addition can be substituted for each other without resulting in ungrammatical sentences are considered to be possible constituents called hypotheses. A system that uses such an approach is ABL (Alignment-Based Learning) [van Zaanen, 2000]. Currently, the main method used to align sentences and produce hypotheses is of such algorithmic complexity that ABL is feasible for small corpora only. This thesis explores the main topics of unsupervised learning of syntactic structure of natural language and introduces new algorithms based on suffix trees. The al- gorithmic complexity of the new algorithms allow ABL to learn from large corpora as well. Furthermore, it shows that the suffix tree data structure has important advan- tages in finding regularities in corpora, which is a fundamental issue in many approaches to unsupervised and semisupervised grammatical inference. The perfor- mance of the new algorithms with respect to a learning task are tested within the ABL framework on corpora of various sizes: the English ATIS, the Dutch OVIS, and the English Wall Street Journal treebank. In conclusion, we observe that the time needed for alignment learning using the new algorithms as a function of the corpus size is indeed reduced in such an extent that learning on large sized corpora with sys- tems like ABL is feasible. However, the recall of the hypothesis constituents introduced by the new algorithms is lower than that of the established algorithm and justifies further research.