The 23-year-old actress has played Lola Pearce on since 2011, but will film her final scenes later this year after being written out of the show, reported Digital Spy.
"I've had the most amazing time at EastEnders having been involved in some exciting storylines, including giving birth in a live scene," said Harold.
"I'll miss everyone here and am looking forward to the future," she added.
Soap boss Dominic Treadwell-Collins added, "We all love Danielle and she and Lola have been a big part of EastEnders over the past four years.
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