Contrary to the conventional emphasis on dataset size, we explore the role of data alignment -- an often overlooked aspect of data quality -- in training capable Large Language Models (LLMs). To do so, we use the Task2Vec-based alignment coefficient, a quantitative measure of the similarity between two datasets, to quantify the impact of alignment between training data and evaluation data on downstream performance. In particular, we conduct controlled \textit{interventional} experiments for two settings: 1. the impact of increased alignment coefficients between various pre-training (pt) against evaluation datasets, and 2. the impact of increased alignment coefficients between domain specific fine-tuning (ft) against domain specific evaluation. The domain specific task we explore is Autoformalization -- the machine translation task between natural language and code for formal verification. In both settings, we find a strong, predictable negative correlation between the alignment coefficient of a model's training and evaluation data and the model's loss/perplexity on the respective downstream task. These findings suggest a re-evaluation of LLM training approaches, demonstrating the relevance of data alignment compared to data quantity, especially in specialized downstream tasks such as Autoformalization.