Alexander excelled at the design of her dolls. "I didn't want to make just ordinary dolls witih unmeaning, empty smiles on their painted lips and a squeaky way of saying 'mama' after you pinched," she said. "I wanted to do dolls with souls. You have no idea how I labored over noses and mouths so that they would look real and individual." To ensure that the dolls' costumes were scrupulously accurate, she returned time and again to the New York Public Library in search of authentic representations of other times, places, and cultures. Her attention to detail was prodigious; even the dolls' petticoats were full and lace-trimmed.

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Standing at the forefront of innovation in doll-making, Alexander experimented constantly to make her dolls more attractive, more lifelike, and more marketable. Dissatisfied with the stiff, flat faces of her cloth dolls, she developed techniques to sculpt in fabric, achieving lively, realistic facial features. Sleep eyes, rooted hair, and walking dolls were among the novelties that emerged from her factory. Having moved from cloth to a new composition material in the 1920s, immediately after World War II she was among the first toy makers to use the new material of plastic, which finally allowed her to fulfill her dream of creating an unbreakable doll.