He was late for work, as although he needed the money, he didn't like the job.
He was late for work. As although he needed the money, he didn't like the job.
Are both of these sentences correct? Can you begin a sentence with as?
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You can begin a sentence with As but, in your specific case, I wouldn't. Although provides better context on its own.
"Although he needed the money" is an afterthought in this sentence – i.e. it is not the reason that he was late. As such, I might rewrite the first sentence as "He was late for work—although he needed the money—he didn't like the job,". Alternatively, I might choose "He was late for work, as he didn't like the job—although he needed the money."
In fairness, not liking the job is not necessarily the reason he was late—it is just how he excuses himself for being so. To that end, depending on the desired flow of your writing, you may prefer to split this into two sentences; the first states that he is late and why, and the second states how he feels about this.
Consider: "He was late for work, as the traffic was busier than he expected. He didn't care; he didn't like the job—although he needed the money." A good editor may tighten that up further, though.