The Black Widow actually trained with the Winter Soldier as far back as the 1950s—she joined her fellow Russian operatives to retrain Bucky Barnes as an agent of the Soviet Union. The two began a brief romance, but the Russians had lingering worries about Bucky’s programming, so they decided to freeze him and thaw him out only when necessary.
After regaining his memories thanks to Captain America and the power of a Cosmic Cube, Bucky also managed to recall his time with Natasha. The heroes restarted their relationship, but the star-crossed lovers were foiled once again when a Russian sleeper agent brainwashed Black Widow, clearing her mind of her relationship with Barnes in the process.
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