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Each of these two leafy colonial neighborhoods is accessible by subway, though you'll need to rely on at least one sitio taxi ride to cover them both in one day. San Angel is closer to the subway than Coyoacán. If you get off the metro at Miguel Angel de Quevedo and walk west down Arenal, you'll soon come to the Monumento al General Alvaro Obregón —the somber, gray, granite monument is a good neighborhood landmark. From there you can easily walk to all the neighborhood's sights with the exception of Museo Casa Estudio Diego Rivera y Frida Kahlo (though if you have the energy, that can technically be reached on foot, too). To start out from the monument, cross Insurgentes to walk up the cobblestoned, restaurant-lined Avenida de la Paz. Next cross Avenida Revolución and take the crooked street that leads upward to the left of the little park until you come to San Angel's center, Plaza San Jacinto.
Coyoacán is farther from the Quevedo stop, but you can reach its main attraction, Museo de Frida Kahlo, on foot. Most of the other sights are within walking distance of the museum, but you'll need a sitio taxi to get to Museo del Anahuacalli.
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