A few points, some echoing what others have said.

First, not to be discouraging, but jobs at the Smithsonian are scarce as
budgets are tight, and there may be more than 100 applicants for many jobs.

Be prepared for the fact that the initial screening will be done by someone
in Personnel who may or may not have any particular knowledge of the job or
what it really requires to do it.  Part of your job in properly filling out
the application paperwork will be to make it through this initial screening.
Be sure to carefully read the job announcement and the selective factors and
quality ranking factors.  Tailor each application you make to the specific
job. It may sound obvious, but try to insert words used in the job
announcement into your application.  If the job is for a curatorial
assistant, even though you may have listed on your resume that you interned
in X museum in x department, it is better not only to mention the internship
but to add, for example, that as part of it you assisted registration and
curatorial staff with putting on an exhibit, just so the words "assisted"
and "curatorial", can be seen by the personnel screener. If a Selective
Factor says: "Knowledge of museum practices and procedures", and you have
not yet actually worked in a museum, then specifically highlight aspects of
your educational, internship or volunteer experiences that could have given
you that knowledge. 

As others have pointed out in general advice to people looking for jobs in
the museum field, the more experience you have, the better off you are, but
the experience does *not* have to be in comparable paid positions.
Internships and volunteer employment in museums *will* be really helpful in
getting you considered for any job, Smithsonian or not. Most Smithsonian
offices are overworked and understaffed, so they want someone who will be
able to hit the ground running.  Previous experience of any kind in the
museum world will be considered a real plus. 

Finally, if you make it past the initial screening process, your application
will be reviewed by the person actually doing the hiring. Again, it may
sound obvious, but make sure the application is neat, grammatical, and
without obvious spelling mistakes. Don't use fancy fonts or try to be too
clever. If your application is succinct and readable, you will already have
gone a long way toward impressing the (usually very busy) person having to
slog through a number of applications.

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