Nah. Dru explained that what vampires call "love" isn't normal, healthy, human love - as depicted, it seems more like ownership of a thing - and, according to the Judge, Angelus lacked any essence of humanity. As Angelus, he literally couldn't love Darla.
As Angel, with a soul, he was capable of feeling something from her, but what he felt was both positive and negative, and the negative was enough stronger than the positive that he was able to stake her the first time. Yes, their bond may have been strengthened in Angel when she started being affected by a soul too, but that was always going to be a fleeting thing.