Labour councillor Lib Peck will stand down from her job as council chief to join the £6.8m unit set up by Sadiq Khan last year to tackle violence across the capital.
Peck's responsibilities will include developing a "long-term partnership strategy" and to ensure "communities and young people are properly represented and consulted".
She will be the point of contact between the unit, and other partner organisations including the Metropolitan Police Service, London boroughs, schools and community groups.
The politician has led the borough council since 2012, and is also the London Councils executive member for crime and public protection.
City Hall said a key focus of the unit is early intervention and "providing young Londoners with better, positive life opportunities".
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